Platinum-ruthenium containing catalyst formulations for hydrogen generation

ABSTRACT

A method and catalysts for producing a hydrogen-rich syngas are disclosed. According to the method a CO-containing gas contacts a water gas shift (WGS) catalyst, optionally in the presence of water, preferably at a temperature of less than about 450° C. to produce a hydrogen-rich gas, such as a hydrogen-rich syngas. Also disclosed is a water gas shift catalyst formulated from:  
     a) Pt, its oxides or mixtures thereof;  
     b) Ru, its oxides or mixtures thereof; and  
     c) at least one of Li, Na, K, Rb, Cs, Mg, Ca, Sr, Ba, Sc, Y, Ti, Zr, V, Mo, Mn, Fe, Co, Rh, Ir, Ge, Sn, Sb, La, Ce, Pr, Sm, and Eu. Another disclosed catalyst formulation comprises Pt, its oxides or mixtures thereof; Ru, its oxides or mixtures thereof; Co, its oxides or mixtures thereof; and at least one of Li, Na, K, Rb, Cs, Mg, Ca, Sr, Ba, Sc, Y, Ti, Zr, V, Mo, Mn, Fe, Rh, Ir, Ge, Sn, Sb, La, Ce, Pr, Sm, and Eu, their oxides and mixtures thereof. The WGS catalyst may be supported on a carrier, such as any one member or a combination of alumina, zirconia, titania, ceria, magnesia, lanthania, niobia, zeolite, perovskite, silica clay, yttria and iron oxide. Fuel processors containing such water gas shift catalysts are also disclosed.

CROSS-REFERENCE TO RELATED APPLICATIONS

[0001] The present application claims benefit from earlier filed U.S.Provisional Application No. 60/434,708, filed Dec. 20, 2002, which isincorporated herein in its entirety by reference for all purposes. Thepresent application also incorporates by reference the PCT InternationalPatent Application No. ______ entitled “Platinum-Ruthenium ContainingCatalyst Formulations for Hydrogen Generation” naming as inventorsHagemeyer et al. (Attorney Docket No. 708000701PCT) filed on the samedate as the present application.

BACKGROUND OF THE INVENTION

[0002] 1. Field of the Invention

[0003] This invention relates to methods and catalysts to generate ahydrogen-rich gas from gas mixtures containing carbon monoxide andwater, such as water-containing syngas mixtures. More particularly, theinvention includes methods using both precious metal- and non-preciousmetal-containing catalysts. The catalysts may be supported on a varietyof catalyst support materials. Catalysts of the invention exhibit bothhigh activity and selectivity to hydrogen generation and carbon monoxideoxidation.

[0004] 2. Discussion of the Related Art

[0005] Numerous chemical and energy-producing processes require ahydrogen-rich composition (e.g. feed stream.) A hydrogen-rich feedstream is typically combined with other reactants to carry out variousprocesses. Nitrogen fixation processes, for example, produce ammonia byreacting feed streams containing hydrogen and nitrogen under highpressures and temperatures in the presence of a catalyst. In otherprocesses, the hydrogen-rich feed stream should not contain componentsdetrimental to the process. Fuel cells such as polymer electrodemembrane (PEM) fuel cells, produce energy from a hydrogen-rich feedstream. PEM fuel cells typically operate with a feed stream gas inlettemperature of less than 450° C. Carbon monoxide is excluded from thefeed stream to the extent possible to prevent poisoning of the electrodecatalyst, which is typically a platinum-containing catalyst. See U.S.Pat. No. 6,299,995.

[0006] One route for producing a hydrogen-rich gas is hydrocarbon steamreforming. In a hydrocarbon steam reforming process steam is reactedwith a hydrocarbon fuel, such as methane, iso-octane, toluene, etc., toproduce hydrogen gas and carbon dioxide. The reaction, shown below withmethane (CH₄), is strongly endothermic; it requires a significant amountof heat.

CH₄+2H₂O→4H₂+CO₂

[0007] In the petrochemical industry, hydrocarbon steam reforming ofnatural gas is typically performed at temperatures in excess of 900° C.Even for catalyst assisted hydrocarbon steam reforming the temperaturerequirement is often still above 700° C. See, for example, U.S. Pat. No.6,303,098. Steam reforming of hydrocarbons, such as methane, usingnickel- and gold-containing catalysts and temperatures greater than 450°C. is described in U.S. Pat. No. 5,997,835. The catalyzed process formsa hydrogen-rich gas, with depressed carbon formation.

[0008] One example of effective hydrocarbon steam reforming catalysts isthe Sinfelt compositions which are composed of Pt, a Group 11 metal, anda Group 8-10 metal. Group 11 metals include Cu, Ag and Au while Group8-10 metals include the other noble metals. These catalyst formulationsare well known in the promotion of hydrogenation, hydrogenolysis,hydrocracking, dealkylation of aromatics, and naphtha reformingprocesses. See, for example, U.S. Pat. Nos. 3,567,625 and 3,953,368. Theapplication of catalysts based on the Sinfelt model to water gas shift(“WGS”) reaction, in particular at conditions suitable for lowertemperature WGS applications such as PEM fuel cells, has not beenpreviously reported.

[0009] Purified hydrogen-containing feed streams have also been producedby filtering the gas mixture produced by hydrocarbon steam reformationthrough hydrogen-permeable and hydrogen-selective membranes. See, forexample, U.S. Pat. No. 6,221,117. Such approaches suffer from drawbacksdue to the complexity of the system and slow flow rates through themembranes.

[0010] Another method of producing a hydrogen-rich gas such as a feedstream starts with a gas mixture containing hydrogen and carbon monoxidewith the absence of any substantial amount of water. For instance, thismay be the product of reforming of a hydrocarbon or an alcohol, andselectively removes the carbon monoxide from that gas mixture. Thecarbon monoxide can be removed by absorption of the carbon monoxideand/or by its oxidation to carbon dioxide. Such a process utilizing aruthenium based catalyst to remove and oxidize the carbon monoxide isdisclosed in U.S. Pat. No. 6,190,430.

[0011] The water gas shift reaction is another mechanism for producing ahydrogen-rich gas but from water (steam) and carbon monoxide. Anequilibrium process, the water gas shift reaction, shown below, convertswater and carbon monoxide to hydrogen and carbon dioxide, and viceversa.

[0012] Various catalysts have been developed to catalyze the WGSreaction. These catalysts are typically intended for use at temperaturesgreater than 450° C. and/or pressures above 1 bar. For instance, U.S.Pat. No. 5,030,440 relates to a palladium and platinum-containingcatalyst formulation for catalyzing the shift reaction at 550-650° C.See also U.S. Pat. No. 5,830,425 for an iron/copper based catalystformulation.

[0013] Catalytic conversion of water and carbon monoxide under water gasshift reaction conditions has been used to produce hydrogen-rich andcarbon monoxide-poor gas mixtures. Existing WGS catalysts, however, donot exhibit sufficient activity at a given temperature to reachthermodynamic equilibrium concentrations of hydrogen and carbon monoxidesuch that the product gas may subsequently be used as a hydrogen feedstream. Specifically, existing catalyst formulations are notsufficiently active at low temperatures, that is, below about 450° C.See U.S. Pat. No. 5,030,440.

[0014] Platinum (Pt) is a well-known catalyst for both hydrocarbon steamreforming and water gas shift reactions. Under typical hydrocarbon steamreforming conditions, high temperature (above 850° C.) and high pressure(greater than 10 bar), the WGS reaction may occur post-reforming overthe hydrocarbon steam reforming catalyst due to the high temperature andgenerally unselective catalyst compositions. See, for instance, U.S.Pat. Nos. 6,254,807, 5,368,835, 5,134,109, and 5,030,440 for a varietyof catalyst compositions and reaction conditions under which the watergas shift reaction may occur post-reforming.

[0015] Metals such as cobalt (Co), ruthenium (Ru), palladium (Pd),rhodium (Rh) and nickel (Ni) have also been used as WGS catalysts butare normally too active for the selective WGS reaction and causemethanation of CO to CH₄ under typical reaction conditions. In otherwords, the hydrogen produced by the water gas shift reaction is consumedas it reacts with the CO present in the presence of such catalysts toyield methane. This methanation reaction activity has limited theutility of metals such as Co, Ru, Pd, Rh and Ni as water gas shiftcatalysts.

[0016] A need exists, therefore, for a method to produce a hydrogen-richgas, such as a hydrogen-rich syngas, and catalysts which are highlyactive and highly selective for both hydrogen generation and carbonmonoxide oxidation at moderate temperatures (e.g. below about 450° C.)to provide a hydrogen-rich syngas from a gas mixture containing hydrogenand carbon monoxide.

SUMMARY OF THE INVENTION

[0017] The invention meets the need for highly active and selectivecatalysts for the generation of hydrogen and the oxidation of carbonmonoxide and to thereby provide a hydrogen-rich gas, such as ahydrogen-rich syngas, from a gas mixture of at least carbon monoxide andwater. Accordingly, the invention provides methods and catalysts forproducing a hydrogen-rich gas.

[0018] The invention is, in a first general embodiment, a method forproducing a hydrogen-rich gas (e.g., syngas) by contacting aCO-containing gas, such as a syngas mixture, with a water gas shiftcatalyst in the presence of water at a temperature of not more than 450°C. In the first general embodiment, the water gas shift catalystcomprises a) Pt, its oxides or mixtures thereof, b) Ru, its oxides ormixtures thereof, and c) at least one member selected from the groupconsisting of Li, Na, K, Rb, Cs, Mg, Ca, Sr, Ba, Sc, Y, Ti, Zr, V, Mo,Mn, Fe, Co, Rh, Ir, Ge, Sn, Sb, La, Ce, Pr, Sm, and Eu, their oxides andmixtures thereof. In another method of the first general embodiment, thewater gas shift catalyst comprises Pt, its oxides or mixtures thereof,Ru, its oxides or mixtures thereof, and at least one member selectedfrom the group consisting of Sc, Y, Ti, V, Mo, Fe, Ir, La, and Ce, theiroxides and mixtures thereof. The catalyst may be supported on a carrier,for example, at least one member selected from the group consisting ofalumina, zirconia, titania, ceria, magnesia, lanthania, niobia, zeolite,perovskite, silica clay, yttria and iron oxide and mixtures thereof. Themethod of the invention may be conducted at a temperature ranging fromabout 150° C. to about 450° C.

[0019] In a second general embodiment, the invention relates to thewater gas shift catalysts themselves—both supported and unsupportedcatalysts. The inventive water gas shift catalyst comprises, in a first,general embodiment, Pt, its oxides or mixtures thereof, Ru, its oxidesor mixtures thereof, and at least one member selected from the groupconsisting of Li, Na, K, Rb, Cs, Mg, Ca, Sr, Ba, Sc, Y, Ti, Zr, V, Mo,Mn, Fe, Co, Rh, Ir, Ge, Sn, Sb, La, Ce, Pr, Sm, and Eu, their oxides andmixtures thereof. In another catalyst of the first general embodiment,the water gas shift catalyst comprises Pt, its oxides or mixturesthereof, Ru, its oxides or mixtures thereof, and at least one memberselected from the group consisting of Sc, Y, Ti, V, Mo, Fe, Ir, La, andCe, their oxides and mixtures thereof. The catalyst may be supported ona carrier comprising at least one member selected from the groupconsisting of alumina, zirconia, titania, ceria, magnesia, lanthania,niobia, zeolite, perovskite, silica clay, yttria and iron oxide andmixtures thereof.

[0020] In a third general embodiment, the invention is directed to theaforementioned water gas shift catalysts of the second generalembodiment in an apparatus for generating a hydrogen gas containingstream from a hydrocarbon or substituted hydrocarbon feed stream. Theapparatus further comprises, in addition to the WGS catalyst, a fuelreformer, a water gas shift reactor, and a temperature controller. Sucha specific WGS apparatus may be located within another larger apparatus,either stationary or otherwise, for generating energy, or a desiredproduct or feed stream, either gaseous or liquid.

[0021] The following described preferred embodiments of the WGS catalystcan be used in each one of the first, second, and third generalembodiments or in specific, related embodiments (e.g., fuel cellreactors, fuel processors, hydrocarbon steam reformers.)

[0022] In one preferred embodiment the water gas shift catalystcomprises Pt, its oxides or mixtures thereof, Ru, its oxides or mixturesthereof, and at least one member selected from the group consisting ofSc, Y, Ti, V, Mo, Fe, Ir, La, and Ce, their oxides and mixtures thereof.

[0023] In a second preferred embodiment the water gas shift catalyst maybe formulated from Pt, its oxides or mixtures thereof, Ru, its oxides ormixtures thereof, Co, its oxides or mixtures thereof and at least one ofK, Cs, V, Mo, Mn, Fe, La, and Ce, their oxides and mixtures thereof.

[0024] In third preferred embodiment the water gas shift catalystcomprises Pt, its oxides or mixtures thereof, Ru, its oxides or mixturesthereof, and at least one of Mo, Fe, and Ce, their oxides and mixturesthereof.

[0025] In yet another preferred embodiment the water gas shift catalystcomprises Pt, its oxides or mixtures thereof, Ru, its oxides or mixturesthereof, Fe, its oxides or mixtures thereof, and optionally Ce, itsoxides or mixtures thereof

BRIEF DESCRIPTION OF THE DRAWINGS

[0026] The patent or application file contains at least one drawingexecuted in color. Copies of this patent or patent applicationpublication with color drawing(s) will be provided by the Office uponrequest and payment of the necessary fee.

[0027] The accompanying drawings, which are included to provide afurther understanding of the invention and are incorporated in andconstitute a part of this specification, illustrate preferredembodiments of the invention and together with the detailed descriptionserve to explain the principles of the invention. In the drawings:

[0028]FIGS. 1A through 1F illustrate the process of producing thelibrary test wafer. The legend for FIG. 1A also applies to FIGS. 1Bthrough 1F exclusively.

[0029]FIGS. 2A through 2F illustrate the process of producing thelibrary test wafer. The legend for FIG. 2A also applies to FIGS. 2Bthrough 2F exclusively.

[0030]FIGS. 3A through 3G illustrate the process of producing thelibrary test wafer. The legend for FIG. 3A also applies to FIGS. 3Bthrough 3G exclusively.

[0031]FIGS. 4A through 4G illustrate the process of producing thelibrary test wafer. The legend for FIG. 4A also applies to FIGS. 4Bthrough 4G exclusively.

[0032]FIGS. 5A through 5H illustrate the process of producing thelibrary test wafer. The legend for FIG. 5A also applies to FIGS. 5Bthrough 5H exclusively.

[0033]FIGS. 6A through 6C illustrate the process of producing thelibrary test wafer, and

[0034]6D through 6H illustrate SpotFire plots of the CO conversionversus CO₂ production for the wafer under WGS conditions at varioustemperatures. The legend for FIG. 6A also applies to FIGS. 6B, and 6Cexclusively.

[0035]FIGS. 7A through 7F illustrate the process of producing a librarytest wafer, and

[0036]7G, 7H and 7I, illustrate SpotFire plots of the CO conversionversus CO₂ production for the wafer under WGS conditions at varioustemperatures. The legend for FIG. 7A also applies to FIGS. 7B through 7Fexclusively.

[0037]FIGS. 8A through 8E illustrate the process of producing a librarytest wafer and 8F, illustrates SpotFire plots of the CO conversionversus CO₂ production for the wafer under WGS conditions. The legend forFIG. 8E also applies to FIGS. 8A through 8D exclusively.

[0038]FIGS. 9A through 9G illustrate the process of producing a librarytest wafer and

[0039]9H, illustrates SpotFire plots of the CO conversion versus CO₂production for the wafer under WGS conditions. The legend for FIG. 9Aalso applies to FIGS. 9B through 9G exclusively.

[0040]FIGS. 10A through 101 illustrate the process of producing alibrary test wafer and

[0041]10J, 10K and 10L, illustrate SpotFire plots of the CO conversionversus CO₂ production for the wafer under WGS conditions at varioustemperatures. The legend for FIG. 11A also applies to FIGS. 10B through10I exclusively.

[0042]FIGS. 11A through 11I illustrate the process of producing alibrary test wafer and

[0043]11J and 11K illustrate SpotFire plots of the CO conversion versusCO₂ production for the wafer under WGS conditions. The legend for FIG.11A also applies to FIGS. 11B through 11I exclusively.

[0044]FIGS. 12A through 12C illustrate plots of the CO concentrationversus temperature for scaled-up catalyst samples under WGS conditionsat various space velocities. The legends for each of FIGS. 12A, 12B, and12C apply to each figure exclusively.

[0045]FIG. 13 illustrates plots of CO concentration versus temperaturefor scaled-up catalyst samples under WGS conditions.

[0046]FIG. 14 illustrates plots of CO concentration versus temperaturefor scaled-up catalyst samples under WGS conditions.

[0047]FIGS. 15A through 15F illustrate the compositional make-up ofvarious exemplary library test wafers.

[0048]FIG. 16A illustrates a representative plot of CO conversion versusCO₂ production for a prototypical library test wafer at varioustemperature,

[0049]16B, illustrates the effect of catalyst selectivity and activityversus the WGS mass balance, and

[0050]16C, illustrates the effect of temperature on catalyst performanceunder WGS conditions.

[0051]FIG. 17 illustrates plots of CO concentration versus temperaturefor scaled-up catalyst samples under WGS conditions.

DETAILED DESCRIPTION OF THE INVENTION

[0052] The invention relates to a method for producing a hydrogen-richgas, such as a hydrogen-rich syngas. According to the method aCO-containing gas such as a syngas contacts a water gas shift catalyst,in the presence of water, preferably a stoichiometric excess of water,preferably at a reaction temperature of less than about 450° C. toproduce a hydrogen-rich gas, such as a hydrogen-rich syngas. Thereaction pressure is preferably not more than about 10 bar. Theinvention also relates to a water gas shift catalyst itself and toapparatus such as water gas shift reactors and fuel processing apparatuscomprising such WGS catalysts.

[0053] A water gas shift catalyst according to the invention comprises:

[0054] a) Pt, its oxides or mixtures thereof;

[0055] b) Ru, its oxides or mixtures thereof; and

[0056] c) at least one member selected from the group consisting of Li,Na, K, Rb, Cs, Mg, Ca, Sr, Ba, Sc, Y, Ti, Zr, V, Mo, Mn, Fe, Co, Rh, Ir,Ge, Sn, Sb, La, Ce, Pr, Sm, and Eu, their oxides and mixtures thereof.The WGS catalyst may be supported on a carrier, such as any one memberor a combination of alumina, zirconia, titania, ceria, magnesia,lanthania, niobia, zeolite, perovskite, silica clay, yttria and ironoxide.

[0057] The WGS catalysts of the invention comprise combinations of atleast three metals or metalloids, selected from at least three groupindicated above, in each and every possible permutation and combination,except as specifically and expressly excluded. Although particularsubgroupings of preferred combinations of metals or metalloids are alsopresented, the present invention is not limited to the particularlyrecited subgroupings.

[0058] Discussion regarding the particular function of variouscomponents of catalysts and catalyst systems is provided herewith solelyto explain the advantage of the invention, and is not limiting as to thescope of the invention or the intended use, function, or mechanism ofthe various components and/or compositions disclosed and claimed. Assuch, any discussion of component and/or compositional function is made,without being bound by theory and by current understanding, unless andexcept such requirements are expressly recited in the claims. Generally,for example, and without being bound by theory, the metals, Pt,component a), and Ru, component b), both have activity as WGS catalysts.The metals or metalloids of component c) may themselves have activity asWGS catalysts, such as Co, but function in combination with either orboth of Pt and Ru to impart beneficial properties to the catalyst of theinvention.

[0059] Catalysts of the invention can catalyze the WGS reaction atvarying temperatures, avoid or attenuate unwanted side reactions such asmethanation reactions, as well as generate a hydrogen-rich gas, such asa hydrogen-rich syngas. The composition of the WGS catalysts of theinvention and their use in WGS reactions are discussed below.

[0060] 1. Definitions

[0061] Water gas shift (“WGS”) reaction: Reaction which produceshydrogen and carbon dioxide from water and carbon monoxide, and viceversa:

[0062] Generally, and unless explicitly stated to the contrary, each ofthe WGS catalysts of the invention can be advantageously applied both inconnection with the forward reaction as shown above (i.e. for theproduction of H₂), or alternatively, in connection with the reversereaction as shown above (i.e., for the production of CO). As such, thevarious catalysts disclosed herein can be used to specifically controlthe ratio of H₂ to CO in a gas stream.

[0063] Methanation reaction: Reaction which produces methane and waterfrom a carbon source, such as carbon monoxide or carbon dioxide, andhydrogen:

[0064] “Syngas” (also called synthesis gas): Gaseous mixture comprisinghydrogen (H₂) and carbon monoxide (CO) which may also contain other gascomponents such as carbon dioxide (CO₂), water (H₂O), methane (CH₄) andnitrogen (N₂).

[0065] LTS: Refers to “low temperature shift” reaction conditions wherethe reaction temperature is less than about 250° C., preferably rangingfrom about 150° C. to about 250° C.

[0066] MTS: Refers to “medium temperature shift” reaction conditionswhere the reaction temperature ranges from about 250° C. to about 350°C.

[0067] HTS: Refers to “high temperature shift” reaction conditions wherethe reaction temperature is more than about 350° C. and up to about 450°C.

[0068] Hydrocarbon: Compound containing hydrogen, carbon, and,optionally, oxygen.

[0069] The Periodic Table of the Elements is based on the present IUPACconvention, thus, for example, Group 9 comprises Co, Rh, and Ir. (Seehttp://www.iupac.org dated May 30, 2002.)

[0070] As discussed herein, the catalyst composition nomenclature uses adash (i.e., “-”) to separate catalyst component groups where a catalystmay contain one or more of the catalyst components listed for eachcomponent group, brackets (i.e., “{ }”) are used to enclose the membersof a catalyst component group, “{two of . . . }” is used if two or moremembers of a catalyst component group are required to be present in acatalyst composition, “blank” is used within the “{ }” to indicate thepossible choice that no additional element is added, and a slash (i.e.,“/”) is used to separate supported catalyst components from theirsupport material, if any. Additionally, the elements within a catalystcomposition formulation include all possible oxidation states, includingoxides, or salts, or mixtures thereof.

[0071] Using this shorthand nomenclature in this specification, forexample, “Pt—{Rh, Ni}—{Na, K, Fe, Os}/ZrO₂” would represent catalystcompositions containing Pt, one or more of Rh and Ni, and one or more ofNa, K, Fe, and Os supported on ZrO₂; all of the catalyst elements may bein any possible oxidation state, unless explicitly indicated otherwise.“Pt—Rh—Ni—{two of Na, K, Fe, Os}” would represent a supported orunsupported catalyst composition containing Pt, Rh, and Ni, and two ormore of Na, K, Fe, and Os. “Rh—{Cu,Ag,Au}—{Na, K, blank}/TiO₂” wouldrepresent catalyst compositions containing Rh, one or more of Cu, Ag andAu, and, optionally, and one of Na or K supported on TiO₂.

[0072] 2. WGS Catalyst

[0073] A water gas shift catalyst of the invention comprises:

[0074] a) Pt, its oxides or mixtures thereof;

[0075] b) Ru, its oxides or mixtures thereof; and

[0076] c) at least one member selected from the group consisting of Li,Na, K, Rb, Cs, Mg, Ca, Sr, Ba, Sc, Y, Ti, Zr, V, Mo, Mn, Fe, Co, Rh, Ir,Ge, Sn, Sb, La, Ce, Pr, Sm, and Eu, their oxides and mixtures thereof.The WGS catalyst may be supported on a carrier, such as any one memberor a combination of alumina, zirconia, titania, ceria, magnesia,lanthania, niobia, zeolite, perovskite, silica clay, yttria and ironoxide.

[0077] In one preferred general embodiment, the water gas shift catalystcomprises Pt, its oxides or mixtures thereof, Ru, its oxides or mixturesthereof, and at least one member selected from the group consisting ofSc, Y, Ti, V, Mo, Fe, Ir, La, and Ce, their oxides and mixtures thereof,and in another preferred general embodiment, the water gas shiftcatalyst comprises Pt, its oxides or mixtures thereof, Ru, its oxides ormixtures thereof, Co, its oxides or mixtures thereof, and at least oneof K, Cs, V, Mo, Mn, Fe, La, and Ce, their oxides and mixtures thereof.Suitable carriers for supported catalysts are discussed below.

[0078] The catalyst components are typically present in a mixture of thereduced or oxide forms; typically one of the forms will predominate inthe mixture. A WGS catalyst of the invention may be prepared by mixingthe metals and/or metalloids in their elemental forms or as oxides orsalts to form a catalyst precursor. This catalyst precursor mixturegenerally undergoes a calcination and/or reductive treatment, which maybe in-situ (within the reactor), prior to use as a WGS catalyst. Withoutbeing bound by theory, the catalytically active species are generallyunderstood to be species which are in the reduced elemental state or inother possible higher oxidation states. The catalyst precursor speciesare believed to be substantially completely converted to thecatalytically active species by the pre-use treatment. Nonetheless, thecatalyst component species present after calcination and/or reductionmay be a mixture of catalytically active species such as the reducedmetal or other possible higher oxidation states and uncalcined orunreduced species depending on the efficiency of the calcination and/orreduction conditions.

[0079] A. Catalyst Compositions

[0080] As discussed above, one embodiment of the invention is a catalystfor catalyzing the water gas shift reaction (or its reverse reaction).According to the invention, a WGS catalyst may have the followingcomposition:

[0081] a) Pt, its oxides and mixtures thereof;

[0082] b) Ru, its oxides and mixtures thereof; and

[0083] c) at least one of Li, Na, K, Rb, Cs, Mg, Ca, Sr, Ba, Sc, Y, Ti,Zr, V, Mo, Mn, Fe, Co, Rh, Ir, Ge, Sn, Sb, La, Ce, Pr, Sm, and Eu, theiroxides and mixtures thereof.

[0084] The amount of each component present in a given catalystaccording to the present invention may vary depending on the reactionconditions under which the catalyst is intended to operate. Generally, aGroup 8, 9 or 10 metal component, may be present in an amount rangingfrom about 0.01 wt. % to about 10 wt. %, preferably about 0.01 wt. % toabout 2 wt. %, and more preferably about 0.05 wt. % to about 0.5 wt. %.The lanthanide elements may be present, typically, in amounts rangingfrom about 0.05 wt. % to about 20 wt. %, preferably about 0.1 wt. % toabout 15 wt. %. The main group and metalloid elements may be present inamounts ranging, generally, from about 0.01 wt. % to about 15 wt. %,preferably about 0.02 wt. % to about 10 wt. %.

[0085] The above weight percentages are calculated on the total weightof the catalyst component in its final state in the catalyst compositionafter the final catalyst preparation step (i.e., the resulting oxidationstate or states) with respect to the total weight of all catalystcomponents plus the support material, if any. The presence of a givencatalyst component in the support material and the extent and type ofits interaction with other catalyst components may effect the amount ofa component needed to achieve the desired performance effect.

[0086] Other WGS catalysts which embody the invention are listed below.Utilizing the shorthand notation discussed above, where each metal maybe present in its reduced form or in a higher oxidation state, thefollowing compositions are examples of preferred catalyst compositions:

Pt—Ru—{Ti, Mo, Fe, Ce}.

Pt—Ru—{V, Mo, Ce}.

Pt—Ru—{V, Mo, Fe}.

Pt—Ru—{Fe, Co, Ir}.

Pt—Ru—{Sc, Y, La, Ce}.

Pt—Ru—Fe—Ce.

Pt—Ru—Ti—{Mo, Fe, Ce}.

[0087] One preferred quaternary catalyst is Pt, Ru, Co and one or moreof K, Cs, V, Mo, Mn, Fe, La, and Ce. Another preferred ternary catalystembodiment is Pt, Ru and one or more of Sc, Y, La, Ce.

[0088] The catalysts may be more advantageously applied in specificoperating temperature ranges. For instance, Pt, Ru and one or more of Laand Ce provides high activity in the LTS temperature range; while Pt,Ru, Fe and Ce, preferably on TiO₂, is preferably utilized in the higherHTS temperature range. For the MTS temperature range, Pt, Ru, Ce and Tion ZrO₂ and Pt, Ru, Fe, Ce on ZrO₂ are particularly preferred. Pt, Ru,Fe on ZrO₂ may be utilized at both MTS and HTS temperature conditionsand provides high selectivity. Titania supported formulations may beutilized advantageously at both LTS and MTS include Pt, Ru, and one ormore of V, Mo and Ce, and at HTS, Pt, Ru, and one or more of V, Mo andFe.

[0089] B. Catalyst Component a): Pt

[0090] A first component in a catalyst of the invention is Pt, componenta). Pt, like all metal components, may be present in a combination ofits reduced forms and its oxides. Catalysts of the invention may containmixtures of these metal states.

[0091] Pt is recognized as a catalyst for the WGS reaction. Typically Ptalone is too active and unselective towards the formation of hydrogenunder typical WGS conditions. However, as demonstrated here, properlymodified Pt containing catalyst formulations may provide both increasedselectivity to hydrogen generation at high activity levels under WGSreaction conditions.

[0092] C. Catalyst Component b): Ru

[0093] Ruthenium and other metals including, for instance, cobalt,palladium, rhodium, and nickel have been used as WGS catalysts but arenormally too active for the selective WGS reaction and cause methanationof CO to CH₄ under typical WGS reaction conditions. In other words, thehydrogen produced by the water gas shift reaction is consumed as itreacts with the CO present in the presence of such catalysts to yieldmethane. This methanation reaction activity has limited the utility ofsuch metals as water gas shift catalysts.

[0094] Unmodified Ru has been shown to catalyze the methanation reactionunder WGS conditions. However, according to the present invention, Rumay be converted to a highly active and selective WGS catalyst byadjusting the Ru loading and alloying with other catalyst componentswhich may moderate the activity of Ru for the methanation reaction. Incombinations of the invention, Pt was found to efficiently alter theselectivity of unmodified Ru. According to the present invention,various dopants may be added to the Pt and Ru containing catalystformulations and some preferred catalysts include, for example,Pt—Ru—Co, Pt—Ru—Fe, Pt—Ru—Ti, Pt—Ru—Co—Fe and Pt—Ru—Ti—V. The resultingcatalyst compositions are highly active and selective WGS catalysts, andexhibit increased selectivity for the WGS reaction over the competingmethanation reaction.

[0095] Pt—Ru compositions can also be gradually moderated, whileenhancing WGS selectivity at the expense of activity, by addingadditional catalyst components such as, for instance, alkali metals,rare earth metals and lanthanides.

[0096] D. Catalyst Component c): “Functional” Metals or Metalloids

[0097] The WGS catalysts of the invention contain at least three metalsor metalloids. In addition to the first two components, discussed above,a WGS catalyst contains metals or metalloids which, when used incombination with Pt and Ru, function to impart beneficial properties tothe catalyst of the invention. A catalyst of the invention, then,further comprises at least one member of Li, Na, K, Rb, Cs, Mg, Ca, Sr,Ba, Sc, Y, Ti, Zr, V, Mo, Mn, Fe, Co, Rh, Ir, Ge, Sn, Sb, La, Ce, Pr,Sm, and Eu, their oxides and mixtures thereof, component c).

[0098] A catalyst of the invention may include Pt and Ru containingcatalysts which may further include activity or selectivity enhancingpromoters such as Ti, V, Mo, Fe, Co, Ge, Sn, Sb, La, Ce, Pr, Sm or Eu.Preferred carriers include, for instance, zirconia, ceria and titania.Preferred supported catalysts include, for example, Pt—Ru—Co—Fe on ZrO₂or TiO₂, Pt—Ru—Co—Na/ZrO₂, Pt—Ru—Ti on ZrO₂ or CeO_(x), and Pt—Ru—Ce—Tion ZrO₂.

[0099] Pt—Ru—Co containing catalyst compositions may preferably compriseone or more of K, Cs, V, Mo, Mn, Fe, La and Ce.

[0100] E. Functional Classification of Catalyst Components

[0101] Without limiting the scope of the invention, discussion of thefunctions of the various catalyst components is offered, along with atemplate for composing catalyst compositions according to the invention.The following classification of various catalyst components will directone of skill in the art in the selection of various catalyst componentsto formulate WGS catalyst compositions according to the presentinvention and depending on the reaction conditions of interest.

[0102] Furthermore, according to the invention, there are severalclasses of catalyst components and metals which may be incorporated intoa water gas shift catalyst. Hence, the various elements recited ascomponents in any of the described embodiments (e.g., as component (c)),may be included in any various combination and permutation to achieve acatalyst composition that is coarsely or finely tuned for a specificapplication (e.g. including for a specific set of conditions, such as,temperature, pressure, space velocity, catalyst precursor, catalystloading, catalyst surface area/presentation, reactant flow rates,reactant ratios, etc.). In some cases, the effect of a given componentmay vary with the operating temperature for the catalyst. These catalystcomponents may function as, for instance, activators or moderatorsdepending upon their effect on the performance characteristics of thecatalyst. For example, if greater activity is desired, an activator maybe incorporated into a catalyst, or a moderator may be replaced by atleast one activator or, alternatively, by at least one moderator onestep further up the “activity ladder.” An “activity ladder” rankssecondary or added catalyst components, such as activators ormoderators, in order of the magnitude of their respective effect on theperformance of a principal catalyst constituent. Conversely, if WGSselectivity of a catalyst needs to be increased (e.g., decrease theoccurrence of the competing methanation reaction), then either anactivator may be removed from the catalyst or, alternatively, thecurrent moderator may be replaced by at least one moderator one stepdown the “activity ladder.” The function of these catalyst component maybe further described as “hard” or “soft” depending on the relativeeffect obtained by incorporating a given component into a catalyst. Thecatalyst components may be metals, metalloids, or even non-metals.

[0103] For instance, typically, a WGS catalyst according to theinvention suitable for use under LTS conditions employs activators andmay only be minimally moderated, if at all, because activation isgenerally the important parameter to be considered under LTS conditions.Such LTS catalysts also may preferably employ high surface area carriersto enhance catalyst activity. Conversely, WGS catalysts used in HTSconditions may benefit from the catalyst being moderated becauseselectivity and methanation are parameters to be considered. Such HTScatalysts may use, for example, low surface area carriers. Accordingly,operating temperature may be considered in selecting a WGS catalystaccording to the present invention for a particular operatingenvironment.

[0104] Activators according to the present invention may include Ru andCo as active and selective WGS-promoting metals. Ir has also beenobserved to have a slight moderating or activating function, dependingon the presence of other counter metals. Other activators may include,but are not limited to, Ti, Zr, V, Mo, La, Ce, Pr and Eu. Ce may be themost active rare earth metal for activating the WGS reaction. La, Pr, Smand Eu may also be active, particularly at lower temperatures. For HTS,Pr and Sm are preferred soft moderators enhancing selectivity withoutsacrificing much activity. For LTS, La and Eu may be useful activators.In general, all lanthanides, other than Ce, show comparable performanceand tend to moderate rather than activate noble metal containingcatalyst systems. Y is a highly selective moderator for HTS systemswhereas La and Eu are active and comparable to Ce for LTS. La is onlyslightly moderating when doping Ce and may therefore be used to adjustthe selectivity of Ce containing catalyst systems.

[0105] Catalyst components that are slightly moderating and highlyselective over a broad temperature range (e.g., a temperature range ofat least about 50° C., preferably at least about 75° C., and mostpreferably a temperature range of at least about 100° C.), where suchtemperature range is included within the overall preferred temperatureranges of up to about 450° C. include Y, Mo, Fe, Pr and Sm; these tendto be selective but not very active at low temperatures, about 250° C.The redox dopants Mo, Fe, Pr and Sm generally lose activity withincreasing pre-reduction temperatures while Fe becomes moderately activeon its own at high WGS reaction temperatures.

[0106] Moderators may also include Ge, Sn and Sb. Typically, formoderators to exert a moderating function, they should be substantiallyin the reduced or metallic state. Ge alloyed with Sn is an example of analloy that was found to be highly active, even for low temperaturesystems, when in the fully oxidized state that is when treated at apre-reduction temperature of about 300° C. which reduces the noblemetals selectively but does not change the active oxidized state of theredox dopants in a catalyst composition.

[0107] E. Supports

[0108] The support or carrier may be any support or carrier used withthe catalyst which allows the water gas shift reaction to proceed. Thesupport or carrier may be a porous, adsorptive, high surface areasupport with a surface area of about 25 to about 500 m²/g. The porouscarrier material may be relatively inert to the conditions utilized inthe WGS process, and may include carrier materials that havetraditionally be utilized in hydrocarbon stream reforming processes,such as, (1) activated carbon, coke, or charcoal; (2) silica or silicagel, silicon carbide, clays, and silicates including those syntheticallyprepared and naturally occurring, for example, china clay, diatomaceousearth, fuller's earth, kaolin, etc.; (3) ceramics, porcelain, bauxite;(4) refractory inorganic oxides such as alumina, titanium dioxide,zirconium oxide, magnesia, etc.; (5) crystalline and amorphousaluminosilicates such as naturally occurring or synthetically preparedmordenite and/or faujasite; and, (6) combinations of these groups.

[0109] When a WGS catalyst of the invention is a supported catalyst, thesupport utilized may contain one or more of the metals (or metalloids)of the catalyst. The support may contain sufficient or excess amounts ofthe metal for the catalyst such that the catalyst may be formed bycombining the other components with the support. Examples of suchsupports include ceria which can contribute cerium, Ce, (component c))to a catalyst, or iron oxide which can contribute iron, Fe, (componentc)). When such supports are used the amount of the catalyst component inthe support typically may be far in excess of the amount of the catalystcomponent needed for the catalyst. Thus the support may act as both anactive catalyst component and a support material for the catalyst.Alternatively, the support may have only minor amounts of a metal makingup the WGS catalyst such that the catalyst may be formed by combiningall desired components on the support.

[0110] Carrier screening with catalysts containing Pt as the only activenoble metal revealed that a water gas shift catalyst may also besupported on a carrier comprising alumina, zirconia, titania, ceria,magnesia, lanthania, niobia, yttria and iron oxide. Perovskite may alsobe utilized as a support for the inventive catalyst formulations.

[0111] Zirconia, titania and ceria may be supports for the presentinvention and provide high activity for the WGS reaction. Preferably,zirconia is in the monoclinic phase. Highly pure ceria was found toactivate PtRuTi in HTS conditions. Niobia, yttria and iron oxidecarriers provide high selectivity but are also less active which isbelieved to be due to a lack of surface area. Pt on magnesia carriersformulated to have high surface areas (approximately 100 m²/g) exhibithigh selectivity but also exhibit activity which decreases rapidly withfalling reaction temperature.

[0112] Iron, yttrium, and magnesium oxides may be utilized as primarylayers on zirconia carriers to provide both higher surface area and lowmoderator concentration.

[0113] In general, alumina has been found to be an active butunselective carrier for Pt only containing WGS catalysts. However, theselectivity of gamma alumina may be improved by doping with Y, Zr, Co,or one of the rare earth elements, such as, for example, La and Ce. Thisdoping may be accomplished by addition of the oxides or other salts suchas nitrates, in either liquid or solid form, to the alumina. Otherpossible dopants to increase the selectivity include redox dopants, suchas for instance, Re, Mo, Fe and basic dopants. Preferred is anembodiment of gamma alumina combined with yttria or with both Zr and/orCo which exhibit both high activity and selectivity over a broadtemperature range.

[0114] High surface area aluminas, such as gamma-, delta-, ortheta-alumina are preferred alumina carriers. Other alumina carriers,such as mixed silica alumina, sol-gel alumina, as well as sol-gel orco-precipitated alumina-zirconia carriers may be used. Alumina typicallyhas a higher surface area and a higher pore volume than carriers such aszirconia and offers a price advantage over other more expensivecarriers.

[0115] F. Methods of Making a WGS Catalyst

[0116] As set forth above, a WGS catalyst of the invention may beprepared by mixing the metals and/or metalloids in their elemental formsor as oxides or salts to form a catalyst precursor, which generallyundergoes a calcination and/or reductive treatment. Without being boundby theory, the catalytically active species are generally understood tobe species which are in the reduced elemental state or in other possiblehigher oxidation states.

[0117] The WGS catalysts of the invention may be prepared by any wellknown catalyst synthesis processes. See, for example, U.S. Pat. Nos.6,299,995 and 6,293,979. Spray drying, precipitation, impregnation,incipient wetness, ion exchange, fluid bed coating, physical or chemicalvapor deposition are just examples of several methods that may beutilized to make the present WGS catalysts. Preferred approaches,include, for instance, impregnation or incipient wetness. The catalystmay be in any suitable form, such as, pellets, granular, bed, ormonolith. See also the co-pending US Patent Application No. ______ filedon the same date as the present application titled “Methods For ThePreparation Of Catalysts For Hydrogen Generation” to Hagemayer et al.under Attorney Docket No. 7080-011-01 for further details on methods ofcatalyst preparation and catalyst precursors. The complete disclosure ofthe above mentioned application and all other references cited hereinare incorporated herein in their entireties for all purposes.

[0118] The WGS catalyst of the invention may be prepared on a solidsupport or carrier material. Preferably, the support or carrier is, oris coated with, a high surface area material onto which the precursorsof the catalyst are added by any of several different possibletechniques, as set forth above and as known in the art. The catalyst ofthe invention may be employed in the form of pellets, or on a support,preferably a monolith, for instance a honeycomb monolith.

[0119] Catalyst precursor solutions are preferably composed of easilydecomposable forms of the catalyst component in a sufficiently highenough concentration to permit convenient preparation. Examples ofeasily decomposable precursor forms include the nitrate, amine, andoxalate salts. Typically chlorine containing precursors are avoided toprevent chlorine poisoning of the catalyst. Solutions can be aqueous ornon-aqueous solutions. Exemplary non-aqueous solvents can include polarsolvents, aprotic solvents, alcohols, and crown ethers, for example,tetrahydrofuran and ethanol. Concentration of the precursor solutionsgenerally may be up to the solubility limitations of the preparationtechnique with consideration given to such parameters as, for example,porosity of the support, number of impregnation steps, pH of theprecursor solutions, and so forth. The appropriate catalyst componentprecursor concentration can be readily determined by one of ordinaryskill in the art of catalyst preparation.

[0120] Li—The acetate, hydroxide, nitrate and formate salts are bothpossible catalyst precursors for lithium.

[0121] Na—Sodium acetate, alkoxides including methoxide, propoxide, andethoxide, bicarbonate, carbonate, citrate, formate, hydroxide, nitrate,nitrite and oxalate may be used to prepare WGS catalysts of theinvention.

[0122] Mg—Water soluble magnesium precursors include the nitrate,acetate, lactate and formate salts.

[0123] K—Potassium nitrate, acetate, carbonate, hydroxide and formateare possible potassium catalyst precursors. The KOAc salt is volatilewith possible potassium losses when heating up to calcinationtemperature.

[0124] Ca—The nitrate, acetate and hydroxide salts, preferable saltshighly soluble in water, may be used to prepare catalysts of theinvention.

[0125] Sc—The nitrate salt, Sc(NO₃)₃ may be a precursor for scandium.

[0126] Ti—Titanium precursors which may be utilized in the presentinvention include ammonium titanyl oxalate, (NH₄)₂TiO(C₂O₄)₂, availablefrom Aldrich, and titanium(IV) bis(ammonium lactato)dihydroxide, 50 wt %solution in water,

[0127] [CH₃CH(O—)CO₂NH₄]₂Ti(OH)₂, available from Aldrich. Other titaniumcontaining precursors include Ti oxalate prepared by dissolving a Ti(IV)alkoxide, such as Ti(IV) propoxide, Ti(OCH₂CH₂CH₃)₄, (Aldrich) in 1Maqueous oxalic acid at 60° C. and stirring for a couple of hours, toproduce a 0.72M clear colorless solution; TiO(acac)oxalate prepared bydissolving Ti(IV) oxide acetylacetonate, TiO(acac)₂, (Aldrich) in 1.5Maqueous oxalic acid at 60° C. with stirring for a couple of hours,following by cooling to room temperature overnight to produce 1M clearyellow-brown solution; TiO(acac)₂, may also be dissolved in diluteacetic acid (50:50 HOAc:H₂O) at room temperature to produce a 1M clearyellow solution of TiO acac. Preferably, titanium dioxide in the anataseform is utilized as a catalyst precursor material.

[0128] V—Vanadium (IV) oxalate, a vanadium precursor, may be preparedfrom V₂O₅, (Aldrich), which is slurried in 1.5M aqueous oxalic acid onhot plate for 1 hour until it turns dark blue due to V(V) reduction toV(IV) by oxalic acid. Ammonium metavanadate(V), (NH₄)VO₃, (Cerac, Alfa)may be used as a precursor by dissolving it in water, preferably hot,about 80° C. water. Various polycarboxylic organic acid vanadiumprecursors can be prepared and used as catalyst precursors, for example,citric, maleic, malonic, and tatartic. Vanadium citrate can be preparedby reacting V₂O₅ with citric acid, and heating to about 80° C. Ammoniumvanadium(V) oxalate may be prepared by reacting (NH₄)VO₃ and NH₄OH inroom temperature water, increasing temperature to 90° C., stirring todissolve all solids, cooling to room temperature and adding oxalic acid;this produces a clear orange solution, which is stable for about 2 days.Ammonium vanadium(V) citrate and ammonium vanadium(V) lactate are bothprepared by shaking NH₄VO₃ in, respectively, aqueous citric acid oraqueous lactic acid, at room temperature. Diammonium vanadium(V) citratemay be prepared by dissolving, for instance, 0.25M NH₄VO₃ in citric aciddiammonium salt (Alfa) at room temperature. An exemplary method ofpreparing ammonium vanadium(V) formate is to dissolve NH₄VO₃ (0.25M) inwater at 95° C., react with 98% formic acid and NH₄OH to produce thedesired ammonium vanadium(V) formate; this method may be utilized toprepare vanadium formate solutions of 0.5 M V concentration or higher.

[0129] Cr—Both the nitrate and acetate hydroxides are possible catalystprecursors for chromium.

[0130] Mn—Manganese nitrate, manganese acetate (Aldrich) and manganeseformate (Alfa) are all possible catalyst precursors for manganese.

[0131] Fe—Iron (III) nitrate, Fe(NO₃)₃, iron(III) ammonium oxalate,(NH₄)₃ Fe(C₂O₄)₃, iron(III) oxalate, Fe₂(C₂O₄)₃, and iron(II) acetate,Fe(OAc)₂, are all water soluble; although the iron(III)oxalate undergoesthermal decomposition at only 100° C. Potassium iron(III) oxalate,iron(III) formate and iron(III) citrate are additional iron precursors.

[0132] Co—Both cobalt nitrate and acetate are water soluble precursorsolutions. The cobalt (II) formate, CO(OOCH)₂, has low solubility incold water of about 5 g/100 ml; while cobalt (II) oxalate is soluble inaqueous NH₄OH. Another possible precursor is sodiumhexanitrocobaltate(III), Na₃Co(NO₂)₆ which is water soluble, withgradual decomposition of aqueous solutions slowed by addition of smallamounts of acetic acid. Hexaammine Co(III) nitrate is also soluble inhot (65° C.) water and NMe₄OH. Cobalt citrate, prepared by dissolvingCo(OH)₂ in aqueous citric acid at 80° C. for 1 to 2 hours, is anothersuitable cobalt precursor.

[0133] Ni—Nickel nitrate, Ni(NO₃)₂, and nickel formate are both possiblenickel precursors. The nickel formate may be prepared by dissolvingNi(HCO₂)₂ in water and adding formic acid, or by dissolving in diluteformic acid, to produce clear greenish solutions.

[0134] Cu—Copper precursors include nitrate, Cu(NO₃)₂, acetate,Cu(OAc)₂, and formate, Cu(OOCH)₂, which are increasingly less watersoluble in the order presented. Ammonium hydroxide is used to solublizeoxalate, Cu(C₂O₄)₂, and Cu(NH₃)₄(OH)₂ which is soluble in aqueous 5NNH₄OH. Copper citrate and copper amine carbonate may be prepared fromCu(OH)₂.

[0135] Zn—Zinc nitrate, acetate and formate are all water soluble andpossible catalyst precursors. Ammonium zinc carbonate, (NH₄)₂Zn(OH)₂CO₃,prepared by reacting zinc hydroxide and ammonium carbonate for a week atroom temperature, is another possible precursor for zinc.

[0136] Ge—Germanium oxalate may be prepared from amorphous Ge(IV) oxide,glycol-soluble GeO₂, (Aldrich) by reaction with 1M aqueous oxalic acidat room temperature. H₂GeO₃ may be prepared by dissolving GeO₂ in waterat 80° C. and adding 3 drops of NH₄OH (25%) to produce a clear,colorless H₂GeO₃ solution. (NMe₄)₂GeO₃ may be prepared by dissolving0.25 M GeO₂ in 0.1 M NMe₄OH. (NH₄)₂GeO₃ may be prepared by dissolving0.25 M GeO₂ in 0.25M NH₄OH.

[0137] Rb—The nitrate, acetate, carbonate and hydroxide salts may beused as catalyst precursors to prepare the WGS catalyst of theinvention. Preferred are water soluble salts.

[0138] Sr—The acetate is soluble in cold water to produce a clearcolorless solution.

[0139] Y—Yttrium nitrate and acetate are both possible catalystprecursors.

[0140] Zr—Zirconyl nitrate and acetate, commercially available fromAldrich, and ammonium Zr carbonate and zirconia, available from MEI, arepossible precursors for zirconium in either or both the support orcatalyst formulation itself

[0141] Nb—Niobium oxalate prepared by dissolving niobium (V) ethoxide inaqueous oxalic acid at 60° C. for 12 hours is a possible catalystprecursor. Another preparative route to the oxalate is dissolving niobicacid or niobic oxide (Nb₂O₅) in oxalic acid at 65° C. Ammonium Nboxalate is also a possible catalyst precursor for niobium. Dissolvingniobic oxide (0.10 M Nb) in NMe₄OH (0.25 M) and stirring overnight at65° C. will produce (NMe₄)₂NbO₆.

[0142] Mo—Molybdenum containing precursor solutions may be derived fromammonium molybdate (NH₄)₂MoO₄ (Aldrich) dissolved in room temperaturewater; Mo oxalate prepared by dissolving MoO₃ (Aldrich) in 1. SM aqueousoxalic acid at 60° C. overnight; and ammonium Mo oxalate prepared from(NH₄)₆Mo₇O₂₄.4H₂O (Strem) dissolved in 1M aqueous oxalic acid at roomtemperature. (NH₄)₆Mo₇O₂₄.4H₂O (Strem) may also be dissolved in water atroom temperature to produce a stable solution of ammonium paramolybdatetetrahydrate. Molybdic acid, H₂MoO₄, (Alfa Aesar or Aldrich) may each bedissolved in room temperature water to produce 1M Mo containingsolutions.

[0143] Ru—Ru nitrosyl nitrate, Ru(NO)(NO₃)₃ (Aldrich), potassiumruthenium oxide, K₂RuO₄.H₂O, potassium perruthenate, KRuO₄, rutheniumnitrosyl acetate, Ru(NO)(OAc)₃, and tetrabutylammonium perruthenate,NBu₄RuO₄, are all possible ruthenium metal catalyst precursors.NMe₄Ru(NO)(OH)₄ solution can be prepared by dissolving Ru(NO)(OH)₃ (0.1M) (H. C. Starck) in NMe₄OH (0.12M) at 80° C. produces a clear darkred-brown 0.1M Ru solution useful as a catalyst precursor solution.

[0144] Rh—A suitable rhodium catalyst precursor is Rh nitrate (Aldrichor Strem).

[0145] Pd—Catalyst compositions containing Pd can be prepared by usingprecursors like Pd nitrate, typically stabilized by dilute HNO₃, andavailable as a 10 wt. % solution from Aldrich, or Pd(NH₃)₂(NO₂)₂available as a 5 wt. % Pd commercial solution, stabilized by diluteNH₄OH. Pd(NH₃)₄(NO₃)₂ and Pd(H₃)₄(OH)₂ are also available commercially.

[0146] Ag—Silver nitrate, silver nitrite, silver diammine nitrite, andsilveracetate are possible silver catalyst precursors.

[0147] Cd—Cadmium nitrate is water soluble and a suitable catalystprecursor.

[0148] In—Indium formate and indium nitrate are preferred precursors forindium.

[0149] Sn—Tin oxalate produced by reacting the acetate with oxalic acidmay be used as a catalyst precursor. Tin tartrate, SnC₄H₄O₆, in NMe₄OHat about 0.25 M Sn concentration, and tin acetate, also dissolved inNMe₄OH at about 0.25 M Sn concentration, may be used as catalystprecursors.

[0150] Sb—Ammonium antimony oxalate produced by reacting the acetatewith oxalic acid and ammonia is a suitable antimony precursor. Antimonyoxalate, Sb₂(C₂O₄)₃, available from Pfaltz & Bauer, is a water solubleprecursor. Potassium antimony oxide, KSbO₃, and antimony citrate,prepared by stirring antimony(II) acetate in 1 M citric acid at roomtemperature, are both possible catalyst precursors.

[0151] Te—Telluric acid, Te(OH)₆, may be used as a precursor fortellurium.

[0152] Cs—Cs salts including the nitrate, acetate, carbonate, andhydroxide are soluble in water and possible catalyst precursors.

[0153] Ba—Barium acetate and barium nitrate are both suitable precursorsfor barium catalyst components.

[0154] La—Lanthanum precursors include nitrate, La(NO₃)₃, acetate,La(OAc)₃, and perchlorate, La(ClO₄)₃, all of which may be prepared asaqueous solutions.

[0155] Ce—Ce(III) and Ce(IV) solutions may be prepared from Ce(III)nitrate hexahydrate, Ce(NO₃)₃.6H₂O, (Aldrich) and ammonium cerium(IV)nitrate, (NH₄)₂Ce(NO₃)₆, (Aldrich), respectively, by dissolution in roomtemperature water. Nitric acid, 5 vol. %, may be added to the Ce(III)salt to increase solubility and stability. Ce(OAc)₃ (Alfa) and Ce(NO₃)₄(Alfa) may also be utilized as catalyst precursors.

[0156] Pr, Nd, Sm and Eu—The nitrate, Ln(NO₃)₃, or acetate, Ln(O₂CCH₃)₃,are possible catalyst precursors for these lanthanides.

[0157] Hf—Hafnoyl chloride and nitrate are both possible precursors.Preparing the hafnoyl nitrate by dissolving Hf(acac)₄ in dilute HNO₃ atlow heat provides a clear stable solution of hafnoyl nitrate.

[0158] Ta—Tantalum oxalate solution, Ta₂O(C₂O₄)₄, available from H. C.Starck, or prepared by dissolving Ta(OEt)₅ in aqueous oxalic acid at 60°C. for 12 hours, is a possible catalyst precursor.

[0159] W—Ammonium metatungstate hydrate, (NH₄)₆W₁₂O₃₉, is water solubleand a possible tungsten catalyst precursor. H₂WO₄ is reacted with NH₄OHand NMe₄OH, respectively, to prepare (NH₄)₂WO₄ and (NMe₄)₂WO₄ which areboth possible precursors.

[0160] Re—Rhenium oxide in H₂O₂, perrhenic acid, (HReO₄), NaReO₄ andNH₄ReO₄ are suitable rhenium precursors.

[0161] Ir—Hexachloroiridate acid, H₂IrCl₆, potassium hexacyanoiridateand potassium hexanitroiridate are all possible catalyst precursors foriridium.

[0162] Pt—Platinum containing catalyst compositions may be prepared byusing any one of a number of precursor solutions, such as,Pt(NH₃)₄(NO₃)₂ (Aldrich, Alfa, Heraeus, or Strem), Pt(NH₃)₂(NO₂)₂, innitric acid, Pt(NH₃)₄(OH)₂ (Alfa), K₂Pt(NO₂)₄, Pt(NO₃)₂, PtCl₄ andH₂PtCl₆ (chloroplatinic acid). Pt(NH₃)₄(HCO₃)₂, Pt(NH₃)₄(HPO₄),(NMe₄)₂Pt(OH)₆, H₂Pt(OH)₆, K₂Pt(OH)₆, Na₂Pt(OH)₆ and K₂Pt(CN)₆ are alsopossible choices along with Pt oxalate salts, such as K₂Pt(C₂O₄)₂. ThePt oxalate salts may be prepared from Pt(NH₃)₄(OH)₂ which is reactedwith 1M oxalic acid solution to produce a clear, colorless solution ofthe desired Pt oxalate salts.

[0163] Au—Auric acid, HAuCl₄, in dilute HCl at about 5% Au may be a goldprecursor. Gold nitrate in 0.1 M concentration may be prepared bydissolving HAu(NO₃)₄ (Alfa) in concentrated nitric acid, followed bystirring at room temperature for 1 week in the dark, then diluting 1:1with water to produce a yellow solution. It should be noted that furtherdilution may result in Au precipitation. More concentrated, 0.25M, forexample, gold nitrate may be prepared by starting with Au(OH)₃ (Alfa).NaAu(OH)₄, KAu(OH)₄, and NMe₄Au(OH)₄ may each be prepared from Au(OH)₃dissolved in bases NaOH, KOH, or NMe₄OH, respectively, in baseconcentrations ranging from, for instance, 0.25 M or higher.

[0164] 3. Producing a Hydrogen-Rich Gas, Such as, a Hydrogen-Rich Syngas

[0165] The invention also relates to a method for producing ahydrogen-rich gas, such as a hydrogen-rich syngas. An additionalembodiment of the invention may be directed to a method of producing aCO depleted gas, such as a CO-depleted syngas.

[0166] A CO-containing gas, such as a syngas contacts with a water gasshift catalyst in the presence of water according to the method of theinvention. The reaction preferably may occur at a temperature of lessthan 450° C. to produce a hydrogen-rich gas such as a hydrogen-richsyngas.

[0167] A method of the invention may be utilized over a broad range ofreaction conditions. Preferably, the method is conducted at a pressureof no more than about 75 bar, preferably at a pressure of no more thanabout 50 bar to produce a hydrogen-rich syngas. Even more preferred isto have the reaction occur at a pressure of no more than about 25 bar,or even no more than about 15 bar, or not more than about 10 bar.Especially preferred is to have the reaction occur at, or aboutatmospheric pressure. Depending on the formulation of the catalystaccording to the present invention, the present method may be conductedat reactant gas temperatures ranging from less than about 150° C. to upto about 450° C. Preferably, the reaction occurs at a temperatureselected from one or more temperature subranges of LTS, MTS and/or HTSas described above. Space velocities may range from about 1 hr⁻¹ up toabout 1,000,000 hr⁻¹. Feed ratios, temperature, pressure and the desiredproduct ratio are factors that would normally be considered by one ofskill in the art to determine a desired optimum space velocity for aparticular catalyst formulation.

[0168] 4. Fuel Processor Apparatus

[0169] The invention further relates to a fuel processing system forgeneration of a hydrogen-rich gas from a hydrocarbon or substitutedhydrocarbon fuel. Such a fuel processing system would comprise, forexample, a fuel reformer, a water gas shift reactor and a temperaturecontroller.

[0170] The fuel reformer would convert a fuel reactant stream comprisinga hydrocarbon or a substituted hydrocarbon fuel to a reformed productstream comprising carbon monoxide and water. The fuel reformer maytypically have an inlet for receiving the reactant stream, a reactionchamber for converting the reactant stream to the product stream, and anoutlet for discharging the product stream.

[0171] The fuel processor system would also comprise a water gas shiftreactor for effecting a water gas shift reaction at a temperature ofless than about 450° C. This water gas shift reactor may comprise aninlet for receiving a water gas shift feed stream comprising carbonmonoxide and water from the product stream of the fuel reformer, areaction chamber having a water gas shift catalyst as described hereinlocated therein, and an outlet for discharging the resultinghydrogen-rich gas. The water gas shift catalyst would preferable beeffective for generating hydrogen and carbon dioxide from the water gasshift feed stream.

[0172] The temperature controller may be adapted to maintain thetemperature of the reaction chamber of the water gas shift reactor at atemperature of less than about 450° C.

5. INDUSTRIAL APPLICATIONS

[0173] Syngas is used as a reactant feed in number of industrialapplications, including for example, methanol synthesis, ammoniasynthesis, oxoaldehyde synthesis from olefins (typically in combinationwith a subsequent hydrogenation to form the corresponding oxoalcohol),hydrogenations and carbonylations. Each of these various industrialapplications preferably includes a certain ratio of H₂ to CO in thesyngas reactant stream. For methanol synthesis the ratio of H₂:CO ispreferably about 2:1. For oxosynthesis of oxoaldehydes from olefins, theratio of H₂:CO is preferably about 1:1. For ammonia synthesis, the ratioof H₂ to N₂ (e.g., supplied from air) is preferably about 3:1. Forhydrogenations, syngas feed streams that have higher ratios of H₂:CO arepreferred (e.g., feed streams that are H₂ enriched, and that arepreferably substantially H₂ pure feed streams). Carbonylation reactionsare preferably effected using feed streams that have lower ratios ofH₂:CO (e.g., feed streams that are CO enriched, and that are preferablysubstantially CO pure feed streams).

[0174] The WGS catalysts of the present invention, and the methodsdisclosed herein that employ such WGS catalysts, can be appliedindustrially to adjust or control the relative ratio H₂:CO in a feedstream for a synthesis reaction, such as methanol synthesis, ammoniasynthesis, oxoaldehyde synthesis, hydrogenation reactions andcarbonylation reactions. In one embodiment, for example, a syngasproduct stream comprising CO and H₂ can be produced from a hydrocarbonby a reforming reaction in a reformer (e.g., by steam reforming of ahydrocarbon such as methanol or naphtha). The syngas product stream canthen be fed (directly or indirectly after further downstream processing)as the feed stream to a WGS reactor, preferably having a temperaturecontroller adapted to maintain the temperature of the WGS reactor at atemperature of about 450° C. or less during the WGS reaction (or atlower temperatures or temperature ranges as described herein inconnection with the catalysts of the present invention). The WGScatalyst(s) employed in the WGS reactor are preferably selected from oneor more of the catalysts and/or methods of the invention. The feedstream to the WGS reactor is contacted with the WGS catalyst(s) underreaction conditions effective for controlling the ratio of H₂:CO in theproduct stream from the WGS reactor (i.e., the “shifted product stream”)to the desired ratio for the downstream reaction of interest (e.g.,methanol synthesis), including to ratios described above in connectionwith the various reactions of industrial significance. As a non-limitingexample, a syngas product stream from a methane steam reformer willtypically have a H₂:CO ratio of about 6:1. The WGS catalyst(s) of thepresent invention can be employed in a WGS reaction (in the forwarddirection as shown above) to further enhance the amount of H₂ relativeto CO, for example to more than about 10:1, for a downstreamhydrogenation reaction. As another example, the ratio of H₂:CO in such asyngas product stream can be reduced by using a WGS catalyst(s) of thepresent invention in a WGS reaction (in the reverse direction as shownabove) to achieve or approach the desired 2:1 ratio for methanolsynthesis. Other examples will be known to a person of skill in the artin view of the teachings of the present invention.

[0175] A person of skill in the art will understand and appreciate thatwith respect to each of the preferred catalyst embodiments as describedin the preceding paragraphs, the particular components of eachembodiment can be present in their elemental state, or in one or moreoxide states, or mixtures thereof.

[0176] Although the foregoing description is directed to the preferredembodiments of the invention, it is noted that other variations andmodifications will be apparent to those skilled in the art, and whichmay be made without departing from the spirit or scope of the invention.

EXAMPLES

[0177] General

[0178] Small quantity catalyst composition samples are generallyprepared by automated liquid dispensing robots (Cavro ScientificInstruments) on flat quartz test wafers.

[0179] Generally supported catalysts are prepared by providing acatalyst support (e.g. alumina, silica, titania, etc.) to the wafersubstrate, typically as a slurry composition using a liquid-handlingrobot to individual regions or locations on the substrate or bywash-coating a surface of the substrate using techniques known to thoseof skill in the art, and drying to form dried solid support material onthe substrate. Discrete regions of the support-containing substrate arethen impregnated with specified compositions intended to operate ascatalysts or catalyst precursors, with the compositions comprisingmetals (e.g. various combinations of transition metal salts). In somecircumstances the compositions are delivered to the region as a mixtureof different metal-containing components and in some circumstances(additionally or alternatively) repeated or repetitive impregnationsteps are performed using different metal-containing precursors. Thecompositions are dried to form supported catalyst precursors. Thesupported catalyst precursors are treated by calcining and/or reducingto form active supported catalytic materials at discrete regions on thewafer substrate.

[0180] The catalytic materials (e.g. supported or bulk) on the substrateare tested for activity and selectivity for the WGS reaction using ascanning mass spectrometer (SMS) comprising a scanning/sniffing probeand a mass spectrometer. More details on the scanning mass spectrometerinstrument and screening procedure are set forth in U.S. Pat. No.6,248,540, in European Patent No. EP 1019947 and in European PatentApplication No. EP 1186892 and corresponding U.S. application Ser. No.09/652,489 filed Aug. 31, 2000 by Wang et al., the complete disclosureof each of which is incorporated herein in its entirety. Generally, thereaction conditions (e.g. contact time and/or space velocities,temperature, pressure, etc.) associated with the scanning massspectrometer catalyst screening reactor are controlled such that partialconversions (i.e., non-equilibrium conversions, e.g., ranging from about10% to about 40% conversion) are obtained in the scanning massspectrometer, for discrimination and ranking of catalyst activities forthe various catalytic materials being screened. Additionally, thereaction conditions and catalyst loadings are established such that theresults scale appropriately with the reaction conditions and catalystloadings of larger scale laboratory research reactors for WGS reactions.A limited set of tie-point experiments are performed to demonstrate thescalability of results determined using the scanning mass spectrometerto those using larger scale laboratory research reactors for WGSreactions. See, for example, Example 12 below.

[0181] Preparative and Testing Procedures

[0182] The catalysts and compositions of the present invention wereidentified using high-throughput experimental technology, with thecatalysts being prepared and tested in library format, as describedgenerally above, and in more detail below. Specifically, such techniqueswere used for identifying catalyst compositions that were active andselective as WGS catalysts. As used in these examples, a “catalystlibrary” refers to an associated collection of candidate WGS catalystsarrayed on a wafer substrate, and having at least two, and typicallythree or more common metal components (including metals in the fullyreduced state, or in a partially or fully oxidized state, such as metalsalts), but differing from each other with respect to relativestoichiometry of the common metal components.

[0183] Depending on the library design and the scope of theinvestigation with respect to a particular library, multiple (i.e., twoor more) libraries were typically formed on each wafer substrate. Afirst group of test wafers each comprised about 100 different catalystcompositions formed on a three-inch wafer substrate, typically with mostcatalysts being formed using at least three different metals. A secondgroup of test wafers each comprised about 225 different catalystcompositions on a four-inch wafer substrate, again typically with mostcatalysts being formed using at least three different metals. Each testwafer itself typically comprised multiple libraries. Each librarytypically comprised binary, ternary or higher-order compositions—thatis, for example, as ternary compositions that comprised at least threecomponents (e.g., A, B, C) combined in various relative ratios to formcatalytic materials having a molar stoichiometry covering a range ofinterest (e.g., typically ranging from about 20% to about 80% or more(e.g. to about 100% in some cases) of each component). For supportedcatalysts, in addition to varying component stoichiometry for theternary compositions, relative total metal loadings were alsoinvestigated.

[0184] Typical libraries formed on the first group of (three-inch) testwafers included, for example, “five-point libraries” (e.g., twentylibraries, each having five different associated catalyst compositions),or “ten-point” libraries (e.g., ten libraries, each having ten differentassociated catalyst compositions), or “fifteen-point libraries” (e.g.,six libraries, each having fifteen different associated catalystcompositions) or “twenty-point libraries” (e.g., five libraries, eachhaving twenty different associated catalyst compositions). Typicallibraries formed on the second group of (four-inch) test wafersincluded, for example, “nine-point libraries” (e.g., twenty-fivelibraries, each having nine different associated catalyst compositions),or “twenty-five point” libraries (e.g., nine libraries, each havingtwenty-five different associated catalyst compositions). Largercompositional investigations, including “fifty-point libraries” (e.g.,two or more libraries on a test wafer, each having fifty associatedcatalyst compositions), were also investigated. Typically, thestoichiometric increments of candidate catalyst library members rangedfrom about 1.5% (e.g. for a “fifty-five point ternary”) to about 15%(e.g., for a “five-point” ternary). See, generally, for example, WO00/17413 for a more detailed discussion of library design and arrayorganization. FIG. 15A to 15F of the instant application shows librarydesigns for libraries prepared on a common test wafer, as graphicallyrepresented using Library Studio® (Symyx Technologies, Inc., SantaClara, Calif.), where the libraries may vary with respect to bothstoichiometry and catalyst loading. Libraries of catalytic materialsthat vary with respect to relative stoichiometry and/or relativecatalyst loading can also be represented in a compositional table, suchas is shown in the several examples of this application.

[0185] Referring to FIG. 15A, for example, the test wafer includes ninelibraries, where each of the nine libraries comprise nine differentternary compositions of the same three-component system. In thenomenclature of the following examples, such a test wafer is said toinclude nine, nine-point-ternary (“9PT”) libraries. The library depictedin the upper right hand corner of this test wafer includes catalystcompositions comprising components A, B and X₁ in 9 differentstoichiometries. As another example, with reference to FIG. 15B, apartial test wafer is depicted that includes a fifteen-point-ternary(“15PT”) library having catalyst compositions of Pt, Pd and Cu infifteen various stoichiometries. Generally, the composition of eachcatalyst included within a library is graphically represented by anassociation between the relative amount (e.g., moles or weight) ofindividual components of the composition and the relative area shown ascorresponding to that component. Hence, referring again to the fifteendifferent catalyst compositions depicted on the partial test waferrepresented in FIG. 155B, it can be seen that each composition includesPt (red), Pd (green) and Cu (blue), with the relative amount of Ptincreasing from column 1 to column 5 (but being the same as comparedbetween rows within a given column), with the relative amount of Pddecreasing from row 1 to row 5 (but being the same as compared betweencolumns within a given row), and with the relative amount of Cudecreasing from a maximum value at row 5, column 1 to a minimum at, forexample, row 1, column 1. FIG. 15C shows a test wafer that includes afifty-point-ternary (“50PT”) library having catalyst compositions of Pt,Pd and Cu in fifty various stoichiometries. This test library could alsoinclude another fifty-point ternary library (not shown), for examplewith three different components of interest.

[0186]FIGS. 15D through 15F are graphical representations of twofifty-point ternary libraries (“bis 50PT libraries”) at various stagesof preparation—including a Pt—Au—Ag/CeO₂ library (shown as the upperright ternary library of FIG. 15E) and a Pt—Au—Ce/ZrO₂ library (shown asthe lower left ternary library of FIG. 15E). Note that the Pt—Au—Ag/CeO₂library also includes binary-impregnated compositions—Pt—Au/CeO₂ binarycatalysts (row 2) and Pt—Ag/CeO₂ (column 10). Likewise, thePt—Au—Ce/ZrO₂ library includes binary-impregnatedcompositions—Pt—Ce/ZrO₂ (row 11) and Au—Ce/ZrO₂ (column 1). Briefly, thebis 50PT libraries were prepared by depositing CeO₂ and ZrO₂ supportsonto respective portions of the test wafer as represented graphically inFIG. 15D. The supports were deposited onto the test wafer as a slurry ina liquid media using a liquid handling robot, and the test wafer wassubsequently dried to form dried supports. Thereafter, salts of Pt, Auand Ag were impregnated onto the regions of the test wafer containingthe CeO₂ supports in the various relative stoichiometries as representedin FIG. 15E (upper-right-hand library). Likewise, salts of Pt, Au and Cewere impregnated onto the regions of the test wafer containing the ZrO₂supports in the various relative stoichiometries as represented in FIG.15E (lower-left-hand library). FIG. 15F is a graphical representation ofthe composite library design, including the relative amount of catalystsupport.

[0187] Specific compositions of tested catalytic materials of theinvention are detailed in the following examples for selected libraries.

[0188] Performance benchmarks and reference experiments (e.g., blanks)were also provided on each quartz catalyst test wafer as a basis forcomparing the catalyst compositions of the libraries on the test wafer.The benchmark catalytic material formulations included a Pt/zirconiacatalyst standard with about 3% Pt catalyst loading (by weight, relativeto total weight of catalyst and support). The Pt/zirconia standard wastypically synthesized by impregnating 3 μL of, for example, 1.0% or 2.5%by weight, Pt stock solution onto zirconia supports on the wafer priorto calcination and reduction pretreatment.

[0189] Typically wafers were calcined in air at a temperature rangingfrom 300° C. to 500° C. and/or reduced under a continuous flow of 5%hydrogen at a temperature ranging from about 200° C. to about 500° C.(e.g., 450° C.). Specific treatment protocols are described below withrespect to each of the libraries of the examples.

[0190] For testing using the scanning mass spectrometer, the catalystwafers were mounted on a wafer holder which provided movement in an XYplane. The sniffing/scanning probe of the scanning mass spectrometermoved in the Z direction (a direction normal to the XY plane of movementfor the wafer holder), and approached in close proximity to the wafer tosurround each independent catalyst element, deliver the feed gas andtransmit the product gas stream from the catalyst surface to thequadrupole mass spectrometer. Each element was heated locally from thebackside using a CO₂ laser, allowing for an accessible temperature rangeof about 2000 to about 600° C. The mass spectrometer monitored sevenmasses for hydrogen, methane, water, carbon monoxide, argon, carbondioxide and krypton: 2, 16, 18, 28, 40, 44 and 84, respectively.

[0191] Catalyst compositions were tested at various reactiontemperatures, typically including for example at about 250° C., 300° C.,350° C. and/or 400° C. Particularly for LTS formulations, testing ofcatalyst activity at reaction temperatures may start as low as 200° C.The feed gas typically consisted of 51.6% H₂, 7.4% Kr, 7.4% CO, 7.4% CO₂and 26.2% H₂O. The H₂, CO, CO₂ and Kr internal standard are premixed ina single gas cylinder and then combined with the water feed. Treatedwater (18.1 mega-ohms-cm at 27.5° C.) produced by a Barnstead Nano PureUltra Water system was used, without degassing.

[0192] Data Processing and Analysis

[0193] Data analysis was based on mass balance plots where CO conversionwas plotted versus CO₂ production. The mass spectrometer signals wereuncalibrated for CO and CO₂ but were based on Kr-normalized massspectrometer signals. The software package SpotFire™ (sold by SpotFire,Inc. of Somerville, Mass.) was used for data visualization.

[0194] A representative plot of CO conversion versus CO₂ production fora WGS reaction is shown in FIG. 16A involving, for discussion purposes,two ternary catalyst systems—a Pt—Au—Ag/CeO₂ catalyst library and aPt—Au—Ce/ZrO₂ catalyst library—as described above in connection withFIGS. 15D through 15F. The catalyst compositions of these libraries werescreened at four temperatures: 250° C., 300° C., 350° C. and 400° C.With reference to the schematic diagram shown in FIG. 16B, active andhighly selective WGS catalysts (e.g., Line I of FIG. 16B) will approacha line defined by the mass balance for the water-gas-shift reaction (the“WGS diagonal”) with minimal deviation, even at relatively highconversions (i.e., at CO conversions approaching the thermodynamicequilibrium conversion (point “TE” on FIG. 16B)). Highly activecatalysts may begin to deviate from the WGS diagonal due to cross-overto the competing methanation reaction (point “M” on FIG. 16C). Catalystcompositions that exhibit such deviation may still, however, be usefulWGS catalysts depending on the conversion level at which such deviationoccurs. For example, catalysts that first deviate from the WGS diagonalat higher conversion levels (e.g., Line II of FIG. 16B) can be employedas effective WGS catalysts by reducing the overall conversion (e.g., bylowering catalyst loading or by increasing space velocity) to theoperational point near the WGS diagonal. In contrast, catalysts thatdeviate from the WGS diagonal at low conversion levels (e.g., Line IIIof FIG. 16B) will be relatively less effective as WGS catalysts, sincethey are unselective for the WGS reaction even at low conversions.Temperature affects the thermodynamic maximum CO conversion, and canaffect the point of deviation from the mass-balance WGS diagonal as wellas the overall shape of the deviating trajectory, since lowertemperatures will generally reduce catalytic activity. For somecompositions, lower temperatures will result in a more selectivecatalyst, demonstrated by a WGS trajectory that more closelyapproximates the WGS mass-balance diagonal. (See FIG. 16C). Referringagain to FIG. 16A, it can be seen that the Pt—Au—Ag/CeO₂ and thePt—Au—Ce/ZrO₂ catalyst compositions are active and selective WGScatalysts at each of the screened temperatures, and particularly atlower temperatures.

[0195] Generally, the compositions on a given wafer substrate weretested together in a common experimental run using the scanning massspectrometer and the results were considered together. In thisapplication, candidate catalyst compositions of a particular library onthe substrate (e.g., ternary or higher-order catalysts comprising threeor more metal components) were considered as promising candidates for anactive and selective commercial catalyst for the WGS reaction based on acomparison to the Pt/ZrO₂ standard composition included on that wafer.Specifically, libraries of catalytic materials were deemed to beparticularly preferred WGS catalysts if the results demonstrated that ameaningful number of catalyst compositions in that library comparedfavorably to the Pt/ZrO₂ standard composition included on the wafersubstrate with respect to catalytic performance. In this context, ameaningful number of compositions was generally considered to be atleast three of the tested compositions of a given library. Also in thiscontext, favorable comparison means that the compositions had catalyticperformance that was as good as or better than the standard on thatwafer, considering factors such as conversion, selectivity and catalystloading. All catalyst compositions of a given library were in many casespositively identified as active and selective WGS catalysts even insituations where only some of the library members compared favorably tothe Pt/ZrO₂ standard, and other compositions within that librarycompared less than favorably to the Pt/ZrO₂ standard. In suchsituations, the basis for also including members of the library thatcompared somewhat less favorably to the standard is that these membersin fact positively catalyzed the WGS reaction (i.e., were effective ascatalysts for this reaction). Additionally, it is noted that suchcompositions may be synthesized and/or tested under more optimally tunedconditions (e.g., synthesis conditions, treatment conditions and/ortesting conditions (e.g., temperature)) than occurred during actualtesting in the library format, and significantly, that the optimalconditions for the particular catalytic materials being tested maydiffer from the optimal conditions for the Pt/ZrO₂ standard—such thatthe actual test conditions may have been closer to the optimalconditions for the standard than for some of the particular members.Therefore, it was specifically contemplated that optimization ofsynthesis, treatment and/or screening conditions, within the generallydefined ranges of the invention as set forth herein, would result ineven more active and selective WGS catalysts than what was demonstratedin the experiments supporting this invention. Hence, in view of theforegoing discussion, the entire range of compositions defined by eachof the claimed compositions (e.g., each three-component catalyticmaterial, or each four-component catalytic material) was demonstrated asbeing effective for catalyzing the WGS reaction. Further optimization isconsidered, with various specific advantages associated with variousspecific catalyst compositions, depending on the desired or requiredcommercial application of interest. Such optimization can be achieved,for example, using techniques and instruments such as those described inU.S. Pat. No. 6,149,882, or those described in WO 01/66245 and itscorresponding U.S. applications, U.S. Ser. No. 09/801,390, entitled“Parallel Flow Process Optimization Reactor” filed Mar. 7, 2001 by Berghet al., and U.S. Ser. No. 09/801,389, entitled “Parallel Flow ReactorHaving Variable Feed Composition” filed Mar. 7, 2001 by Bergh et al.,each of which are incorporated herein by reference for all purposes.

[0196] Additionally, based on the results of screening of initiallibraries, selective additional “focus” libraries were selectivelyprepared and tested to confirm the results of the initial libraryscreening, and to further identify better performing compositions, insome cases under the same and/or different conditions. The test wafersfor the focus libraries typically comprised about 225 differentcandidate catalyst compositions formed on a four-inch wafer substrate,with one or more libraries (e.g. associated ternary compositions A, B,C) formed on each test wafer. Again, the metal-containing components ofa given library were typically combined in various relative ratios toform catalysts having stoichiometry ranging from about 0% to about 100%of each component, and for example, having stoichiometric increments ofabout 10% or less, typically about 2% or less (e.g., for a “fifty-sixpoint ternary”). Focus libraries are more generally discussed, forexample, in WO 00/17413. Such focus libraries were evaluated accordingto the protocols described above for the initial libraries.

[0197] The raw residual gas analyzer (“rga”) signal values generated bythe mass spectrometer for the individual gases are uncalibrated andtherefore different gases may not be directly compared. Methane data(mass 16) was also collected as a control. The signals are typicallystandardized by using the raw rga signal for krypton (mass 84) to removethe effect of gas flow rate variations. Thus, for each library element,the standardized signal is determined as, for example, sH₂O=raw H₂O/rawKr; sCO=raw CO/raw Kr; sCO₂=raw CO₂/raw Kr and so forth.

[0198] Blank or inlet concentrations are determined from the average ofthe standardized signals for all blank library elements, i.e. libraryelements for which the composition contains at most only support. Forexample, b_(avg) H₂O=average sH₂O for all blank elements in the library;b_(avg) CO=average sCO for all blank elements in the library; and soforth.

[0199] Conversion percentages are calculated using the blank averages toestimate the input level (e.g., b_(avg) CO) and the standardized signal(e.g., sCO) as the output for each library element of interest. Thus,for each library element, CO_(conversion)=100×(b_(avg) CO−sCO)/b_(avg)CO and H₂CO_(conversion)=100×(b_(avg) H₂O−sH₂O)/b_(avg) H₂O.

[0200] The carbon monoxide (CO) to carbon dioxide (CO₂) selectivity isestimated by dividing the amount of CO₂ produced (sCO₂−b_(avg) CO₂) bythe amount of CO consumed (b_(avg) CO−sCO). The CO₂ and CO signals arenot directly comparable because the rga signals are uncalibrated.However, an empirical conversion constant (0.6 CO₂ units=1 CO unit) hasbeen derived, based on the behavior of highly selective standardcatalyst compositions. The selectivity of the highly selective standardcatalyst compositions approach 100% selectivity at low conversion rates.Therefore, for each library element, estimated CO to CO₂selectivity=100×0.6×(sCO₂−b_(avg) CO₂)/(b_(avg) CO−sCO). Low COconsumption rates can produce highly variable results, and thus thereproducibility of CO₂ selectivity values is maintained by artificiallylimiting the CO₂ selectivity to a range of 0 to 140%.

[0201] The complete disclosure of all references cited herein areincorporated herein in their entireties for all purposes.

[0202] The following examples are representative of the screening oflibraries that lead to identification of the particularly claimedinventions herein.

Example 1

[0203] A 6.8% Pt/titania masterbatch was prepared by incipient wetnessimpregnation of 1000 mg titania powder (Degussa Aerolyst 7708, less than100 mesh sieve fraction) with 1,300 μl of Pt(NH₃)₂(NO₂)₂ stock solution(5% Pt, STREM) and dried overnight at ambient, then at 80° C., then at110° C.

[0204] 500 mg of the 6.8% Pt/TiO₂ masterbatch was slurried into 4 ml ofEG/H₂O/MEO 40/30/30 mixture and then slurry-dispensed onto a 3″ quartzwafer in two layers of 3 μl slurry each for a total dispense volume of 6μl.

[0205] The Pt/TiO₂ precoated wafer was then impregnated with 25different metal solutions in squares of 2 by 2 wells by directdispensing from metal stock solution vials onto the wafer at 2 μldispense volume/well. The wafer was dried, calcined in air at 450° C.for 2 hours and then reduced in 5% H₂/Ar at 450° C. for 2 hours. SeeFIGS. 1A-1F.

[0206] The reduced library was then screened in scanning massspectrometer (“SMS”) for WGS activity with a H₂/CO/CO₂/H₂O mixed feed at250° C., 300° C., 350° C., and 400° C. This set of experimentsdemonstrated active and selective WGS catalyst formulations of Pt withvarious metals on TiO2 support.

Example 2

[0207] A 3″ quartz wafer was precoated with TiO₂, CeO₂ and ZrO₂ carriersby slurry dispensing (Degussa Aerolyst 7711/Degussa P25 70:30 titaniamix), (Aldrich ceria 21,157-5) and (Norton XZ16052/MEI FZO923 70:30zirconia mix) onto the wafer.

[0208] The carrier-precoated wafer was dried and then impregnated withRu, Ce, Fe gradients. The Ru, Ce, Fe gradients were premixed in amicrotiter plate by dilution of Ru nitrosyl nitrate stock solution (1.5%Ru), Ce nitrate stock solution (1M Ce) and Fe nitrate stock solution (1MFe) with water and transferred from the microtiter plate to the wafer byCavro dispensing (3 μl dispense volume per well). The wafer was driedand then impregnated with Ti gradients. The Ti gradients were premixedin a microtiter plate by dilution of ammonium titanyl oxalate stocksolution (1M Ti) with water and then transferred from the microtiterplate to the wafer by Cavro dispensing (3 μl dispense volume per well).The wafer was dried and then impregnated with Pt gradients. The Ptgradients were premixed in a microtiter plate by dilution ofPt(NH₃)₂(NO₂)₂ stock solution (5% Pt) with water and then transferredfrom the microtiter plate to the wafer by Cavro dispensing (3 μldispense volume per well). The wafer was dried, calcined in air at 500°C. for 1 hour and then reduced in 5% H₂/Ar at 300° C. for 4 hours. SeeFIGS. 2A-2E.

[0209] The reduced library was then screened in SMS for WGS activitywith a H₂/CO/CO₂/H₂O mixed feed at 250° C., 300° C., 350° C., and 400°C. This set of experiments demonstrated active and selective WGScatalyst formulations of Pt—Ce—Fe containing formulations on ZrO₂ andTiO₂ supports.

Example 3

[0210] A 4″ quartz wafer was precoated with zirconia carrier by repeatedslurry dispensing zirconia (ZrO₂ Norton XZ16052/MEI FZO923 70:30mixture, 2×4 μl for a total of 8 μl zirconia slurry, 1 g ZrO₂ mixslurried in 4 ml EG/H₂O 1:1) onto the wafer.

[0211] The zirconia carrier-precoated wafer was dried and thenimpregnated with Pt by Cavro dispensing from a Pt(NH₃)₂(NO₂)₂ stocksolution vial (2.5% Pt) directly onto the wafer by 3 μl dispensevolume/well. Six internal standards were spotted into 6 first row/lastcolumn wells (4 μl zirconia slurry+3 μl 2.5% Pt solution). The wafer wasdried for 10 minutes at 70

[0212] The wafer was then impregnated with Co—Ru and Ru—Pt gradients byCavro dispensing from Co nitrate (0.5M Co), Ru nitrosyl nitrate (1% Ru)and Pt(NH₃)₂(NO₂)₂ (5% Pt) stock solution vials to a microtiter platefollowed by transferring replicas of the 8-point and 7-point gradientsonto the wafer at 3 μl dispense volume/well. The wafer was dried andthen impregnated with FeCo by Cavro dispensing from Fe nitrate (1M Fe)and Co nitrate (0.5M Co) stock solution vials to a microtiter plate(8-point and 7-point gradients) followed by transferring replicas of theFe—H₂O and Fe—Co gradients onto the wafer, 3 μl dispense volume perwell. The wafer was dried and then impregnated with Pt by Cavrodispensing from a Pt(NH₃)₂(NO₂)₂ stock solution vial (2.5% Pt) directlyonto the wafer by 3 μl dispense volume/well.

[0213] Thus four sub-libraries: 8×8 quaternary PtRuCoFe (Pt first) and8×7 quaternary PtRuCoFe (Pt last, to check the effect of order of Ptaddition) and 7×8 ternary RuCoFe and 7×7 quaternary PtRuCoFe are mappedout as rectangles/squares with orthogonal gradients. The wafer wasdried, calcined in air at 500° C. for 1 hour and then reduced in 5%H₂/Ar at 400° C. for 3 hours. A commercial catalyst was slurried into 5positions of the first row and last column as external standards (3 μlcatalyst slurry). See FIGS. 3A-3G.

[0214] The reduced library was then screened in SMS for WGS activitywith a H₂/CO/CO₂/H₂O mixed feed at 250° C., 300° C., 350° C., and 400°C. This set of experiments demonstrated active and selective WGScatalyst formulations of Pt—Ru—Co—Fe and Pt-free Ru—Co—Fe compositions.

Example 4

[0215] A 4″ quartz wafer was precoated with ZrO₂ carrier by slurrydispensing 3 μl of mixed zirconia powder slurry (Norton ZrO₂ XZ16052/MEIZrO₂ FZO923 70:30, 1.5 g ZrO₂/4 ml MEO/EG/H₂O 50:25:25).

[0216] The zirconia carrier precoated wafer was impregnated with {Sc, Y,La, Ce} gradients by Cavro dispensing from Sc, Y, La, Ce nitrate stocksolution vials to a microtiter plate (single column 7-point and 8-pointgradients) followed by transferring replicas of the four 7P and 8Pcolumns onto the wafer (2.5 μl dispense volume per well, 8 replicas ofthe 7PCs and 7 replicas of the 8PCs). Six internal standards were alsosynthesized by spotting 3 μl of a Pt(NH₃)₂(NO₂)₂ stock solution (2.5%Pt) into the corresponding first row/last column positions. The waferwas slowly dried at room temperature and then impregnated with Rugradient by Cavro dispensing from Ru nitrosyl nitrate stock solutionvial to microtiter plate (single row 8-point and 7-point gradients;water vial in Pt position) followed by transferring replicas of the 7Pand 8P row onto the wafer (2.5 μl dispense volume per well, 16 replicasof the 7PR gradient and 14 replicas of the 8PR gradient, 7×8=56 pointternaries, four 56PT on the wafer). The wafer was slowly dried at roomtemperature and then impregnated with Pt gradient by Cavro dispensingfrom Pt(NH₃)₂(NO₂)₂ stock solution vial to microtiter plate (single row8-point and 7-point gradients; water vial in Ru position) followed bytransferring replicas of the 7P and 8P row onto the wafer (2.5 μldispense volume per well, 16 replicas of the 7PR gradient and 14replicas of the 8PR gradient, 7×8=56 point ternaries, four 56PT on thewafer). The wafer was dried and then calcined in air at 500° C. for 1hour followed by reduction with 5% H₂/N₂ at 400° C. for 2 hours.Commercial catalyst was slurried into 5 positions of the first row andlast column as external standards (3 μl catalyst slurry/well). See FIGS.4A-4G.

[0217] The reduced library was then screened in SMS for WGS activitywith a H₂/CO/CO₂/H₂O mixed feed at 250° C., 300° C. and 350° C. This setof experiments demonstrated active and selective WGS catalystformulations of Pt—Ru—{La, Ce} at MTS and HTS reaction conditions.

Example 5

[0218] A 4″ quartz wafer was precoated with ZrO₂ carrier by slurrydispensing 3 μl of mixed zirconia powder slurry (Norton ZrO₂ XZ16052/MEIZrO₂ FZO923 70:30, 1.5 g ZrO₂/4 ml MEO/EG/H₂O 50:25:25).

[0219] The zirconia carrier precoated wafer was impregnated with Cogradients by Cavro dispensing from Co nitrate stock solution vial tomicrotiter plate (single column 7-point and 8-point Co gradients)followed by transferring replicas of the 7P and 8P column onto the wafer(2.5 μl dispense volume per well, 16 replicas of the 7PC and 14 replicasof the 8PC). The wafer was slowly dried at room temperature and thenimpregnated with Ru gradients by Cavro dispensing from Ru nitrosylnitrate stock solution vial to microtiter plate (single row 8-point and7-point Ru gradients) followed by transferring replicas of the 7P and 8Prow onto the wafer (2.5 μl dispense volume per well, 16 replicas of the7PR gradient and 14 replicas of the 8PR gradient, 7×8=56 pointternaries, four 56PT on the wafer). Six internal standards were alsosynthesized by spotting 3 μl of Pt(NH₃)₂(NO₂)₂ stock solution (2.5% Pt)into the corresponding first row/last column positions. The wafer wasslowly dried at room temperature and then impregnated with K by Cavrodispensing 2.5 μl/well from 0.2M KNO₃ tock solution vial directly ontothe lower half of the wafer. The wafer was dried and then impregnatedwith Pt by Cavro dispensing 2.5 μl/well from Pt(NH₃)₂(NO₂)₂ stocksolution vials directly onto the wafer (left hand side of waferuniformly impregnated with 1% Pt solution and right hand side uniformlyimpregnated with 2% Pt solution). The wafer was slowly dried at roomtemperature, calcined in air at 450° C. for 2 hours and then reduced ina flow of 5% H₂/N₂ at 400° C. for 2 hours. Commercial catalyst wasslurried into 5 positions of the first row and last column as externalstandards (3 μl catalyst slurry/well). See FIGS. 5A-5H.

[0220] The reduced library was then screened in SMS for WGS activitywith a H₂/CO/CO₂/H₂O mixed feed at 250° C., 300° C. and 350° C. This setof experiments demonstrated active and selective WGS catalystformulations of Pt—Ru—Co compositions.

Example 6

[0221] A 3″ quartz wafer was coated with niobia, ceria and magnesiacarriers by slurry-dispensing aqueous carrier slurries onto the wafer (4μl slurry/well, 1 g of carrier powder slurried in 2 ml H₂O for niobiaand ceria; 500 mg of carrier powder slurried in 2 ml H₂O for magnesia).Niobia carriers were produced by Norton, product numbers 2001250214,2000250356, 2000250355, 2000250354 and 2000250351. Cerias came fromNorton (product numbers 2001080053, 2001080052 and 2001080051) andAldrich (product number 21,157-50. Magnesia was obtained from Aldrich(product number 24,338-8).

[0222] The carrier precoated wafer was then loaded with the same Ptgradient for each carrier in a single impregnation step by liquiddispensing 3 μl Pt(NH₃)₂(NO₂)₂ solution (5% Pt) from microtiter plate towafer. The wafer was dried and then reduced in 5% H₂/Ar at 450° C. for 2hours. See FIGS. 6A through 6C.

[0223] The reduced library was then screened in SMS for WGS activitywith a H₂/CO/CO₂/H₂O mixed feed at 250° C., 300° C., 350° C., and 400°C. Results at 250° C., 300° C., 350° C., and 400° C. are presented inFIGS. 6D through 6H.

[0224] This set of experiments demonstrated active and selective WGScatalyst formulations of various Pt on one of Nb oxide, Ce oxide or Mgoxide formulations on the wafer. Various Norton niobia carriers werefound to be very active and selective over a broad temperature range.Norton ceria 2001080051 was found to be very selective at highertemperatures. Magnesia was less active than either of niobia or ceriabut did exhibit highly selective WGS performance.

Example 7

[0225] A 4″ quartz wafer was coated with fourteen different catalystcarriers by slurry-dispensing the carrier slurries onto the wafer. Eachwafer column was coated with a different carrier, except for columns 14and 15 which were both coated with gamma-alumina, described below:

[0226] Ceria, 99.5% purity; 9 to 15 nm particle size; BET (m²/g): 55-95;Alfa 43136; dispensed onto the wafer from a slurry of 0.75 g powderslurried in 4 mL ethylene glycol (“EG”)/H₂O/MEO 40:30:30 mixture.

[0227] Ceria, produced by the low temperature calcination ofprecipitated Ce hydroxide; dispensed onto the wafer from a slurry of 1.5g powder slurried in 4 mL EG/H₂O/MEO 40:30:30 mixture.

[0228] Zirconia; 99.8% purity; BET (m²/g): greater than 90; NortonXZ16052; dispensed onto the wafer from a slurry of 1.5 g powder slurriedin 4 mL EG/H₂O/MEO 40:30:30 mixture.

[0229] Zirconia; 99.8% purity; BET (m²/g): 269; Norton XZ16154;dispensed onto the wafer from a slurry of 1.5 g powder slurried in 4 mLEG/H₂O/MEO 40:30:30 mixture.

[0230] Titania; BET (m²/g): 45; Degussa Aerolyst 7708; dispensed ontothe wafer from a slurry of 1.0 g powder slurried in 4 mL EG/H₂O/MEO40:30:30 mixture.

[0231] Titania; 99% purity; BET (m²/g): 37; Norton XT25384; dispensedonto the wafer from a slurry of 1.0 g powder slurried in 4 mL EG/H₂O/MEO40:30:30 mixture.

[0232] Niobia; 97% purity; BET (m²/g): 27; Norton 355; dispensed ontothe wafer from a slurry of 1.0 g powder slurried in 4 mL EG/H₂O/MEO40:30:30 mixture.

[0233] Lanthania; 99.999% purity; Gemre-5N from Gemch Co., Ltd.(Shanghai, China); dispensed onto the wafer from a slurry of 1.5 gpowder slurried in 4 mL EG/H₂O/MEO 40:30:30 mixture.

[0234] Mixed Fe—Ce—O; coprecipitated Fe and Ce oxalate; calcined at 360°C.; dispensed onto the wafer from a slurry of 1.0 g powder slurried in 4mL EG/H₂O/MEO 40:30:30 mixture.

[0235] Mixed La—Ce—O; coprecipitated La and Ce oxalate; calcined at 760°C.; dispensed onto the wafer from a slurry of 1.0 g powder slurried in 4mL EG/H₂O/MEO 40:30:30 mixture.

[0236] Mixed Sb₃O₄—SnO₂ carrier from Alfa; 99.5% purity; BET (m²/g):30-80; Sb₃O₄:SnO₂ ratio is 10:90 by weight; dispensed onto the waferfrom a slurry of 1.0 g powder slurried in 4 mL EG/H₂O/MEO 40:30:30mixture.

[0237] Mixed Fe—Cr—Al—O; commercially available high temperature watergas shift catalyst; dispensed onto the wafer from a slurry of 1.0 powderslurried in 4 mL EG/H₂O/MEO 40:30:30 mixture.

[0238] Fe₂O₃/FeOOH; BET (m²/g): 14; 50:50 physical mixture of commercialpowders (Bayferrox 720N: Bayoxide E3920 from Bayer); dispensed onto thewafer from a slurry of 1.0 g powder slurried in 4 mL EG/H₂O/MEO 40:30:30mixture.

[0239] 14 and 15) Gamma-Al₂O₃; BET (m²/g): 150; Condea Catalox Sba150;dispensed onto the wafer from a slurry of 1.0 g powder slurried in 4 mLEG/H₂O/MEO 40:30:30 mixture.

[0240] In all cases, except for carrier 1, the slurries were applied in3 μL per well; carrier 1 was deposited as two aliquots of 3 μl/well. Thewafer was then dried at 70° C. for 10 minutes.

[0241] Columns 14 and 15 were coated with 2.5 L per well of zirconylnitrate (0.25M) and lanthanum nitrate (0.25M), respectively, then driedfor 10 minutes at 70° C. The first 13 columns of the carrier coatedwafer were then loaded with a 15 point Pt gradient by liquid dispensingof 3 μL Pt(NH₃)₂(NO₂)₂ solution (1% Pt) from microtiter plate to wafer.The wafer was dried at 70° C. for 10 minutes. Columns 14 and 15 werethen loaded with a 15 point Pt gradient by liquid dispensing of 3 μLPt(NH₃)₂(NO₂)₂ solution (1% Pt) from microtiter plate to wafer. Thewafer was dried at 70° C. for 10 minutes, calcined in air at 350° C. for2 hours, then reduced in 5% H₂/Ar at 450° C. for 2 hours. Six internalstandards were synthesized by spotting 3 μL Pt(NH₃)₂(NO₂)₂ solution(1.0% Pt) into the corresponding first row/last column positions. SeeFIGS. 7A through 7F.

[0242] The reduced library was then screened in SMS for WGS activitywith a H₂₁CO/CO₂/H₂O mixed feed at 250° C. and 300° C. The CO conversionversus CO₂ production results at 250° C. and 300° C. are presented inFIGS. 7G, 7H and 71. More detailed test results, such as, CO conversion,CO₂ production and CH₄ production at 250° C. and 300° C. for each of the225 individual catalyst wells on the test wafer are presented in Table1.

[0243] This set of experiments demonstrated active and selective WGScatalyst formulations of various Pt on various of the oxide carrierformulations on the wafer.

Example 8

[0244] A 4″ quartz wafer was precoated with zirconia carrier by repeatedslurry dispensing zirconia powder (Norton XZ16052) onto the wafer. Theslurry was composed of 1.5 g zirconia powder in 4 mL of a MEO/EG/H₂O40:30:30 mixture. A total of 3 μL of slurry was deposited on each spot.

[0245] The zirconia carrier precoated wafer was impregnated withconcentration gradients of Ru—Co, Ru—Ce, Ru—La and Ru—La solution byCavro dispensing from metal stock solutions vials to a microtiter platefollowed by transferring replicas of the 8 col.×7P, 7 col.×8P, 8col.×7P, and 7 col.×8P gradients, respectively, onto the wafer (2.5 μldispense volume per well). Co, Ce and La were provided as theirnitrates, Zr as the zirconyl nitrate and Ru as the nitrosyl nitrate. Thewafer was dried at 70° C. for 10 minutes and then was uniformly coatedwith 2.5 μl/well of a Pt(NH₃)₂(NO₂)₂ stock solution (1% Pt).

[0246] The wafer was dried at 70° C. for 10 minutes, calcined in air at350° C. for 2 hours, then reduced in 5% H₂/Ar at 300° C. for 2 hours.Seven internal standards were synthesized by spotting 2.5 μlPt(NH₃)₂(NO₂)₂ solution (1.0% Pt) into the corresponding first row/lastcolumn and center positions. See FIGS. 8A through 8E.

[0247] The reduced library was then screened in SMS for WGS activitywith a H₂/CO/CO₂/H₂O mixed feed at 300° C. The CO conversion versus CO₂production results at 300° C. are presented in FIG. 8F. More detailedtest results, such as, CO conversion, CO₂ production and CH₄ productionat 300° C. for each of the 225 individual catalyst wells on the testwafer are presented in Table 2.

[0248] This set of experiments demonstrated active and selective WGScatalyst formulations of Pt—Ru—{Co, Ce, La, Zr} compositions on thewafer.

Example 9

[0249] A 4″ quartz wafer was precoated with zirconia carrier by repeatedslurry dispensing zirconia powder (Norton XZ16052) onto the wafer. Theslurry was composed of 1.5 g zirconia powder in 4 mL of a MEO/EG/H₂O40:30:30 mixture. A total of 3 μL of slurry was deposited on each spot.

[0250] The zirconia carrier precoated wafer was impregnated withconcentration gradients of Ti, Zr, Fe and La solution by Cavrodispensing from metal stock solutions vials to a microtiter platefollowed by transferring replicas of the 8P Ti, 7P Zr, 8P Fe and 7P Lagradients, respectively, onto the wafer (2.5 μl dispense volume perwell). Fe and La were provided as their nitrates, Zr as the zirconylnitrate and Ti as the ammonium titanyl oxalate. The wafer was dried at70° C. for 10 minutes and then a 7P and 8P×2 gradient of Ru, as thenitrosyl nitrate was transferred from a microtiter plate to the wafer(2.5 μl dispense volume/well.) The wafer was dried at 70° C. for 10minutes and then was uniformly coated with 2.5 μl/well of aPt(NH₃)₂(NO₂)₂ stock solution (1% Pt).

[0251] The wafer was dried at 70° C. for 10 minutes, calcined in air at450° C. for 2 hours, then reduced in 5% H₂/Ar at 450° C. for 2 hours.Seven internal standards were synthesized by spotting 2.5 μlPt(NH₃)₂(NO₂)₂ solution (1.0% Pt) into the corresponding first row/lastcolumn and center positions. See FIGS. 9A through 9G.

[0252] The reduced library was then screened in SMS for WGS activitywith a H₂/CO/CO₂/H₂O mixed feed at 250° C. and 300° C. The CO conversionversus CO₂ production results at 350° C. are presented in FIG. 9H. Moredetailed test results, such as, CO conversion, CO₂ production and CH₄production at 350° C. for each of the 225 individual catalyst wells onthe test wafer are presented in Table 3.

[0253] This set of experiments demonstrated active and selective WGScatalyst formulations of Pt—Ru—{Ti, Zr, Ti, Fe} compositions on thewafer.

Example 10

[0254] A 4″ quartz wafer was precoated with zirconia carrier by repeatedslurry dispensing zirconia powder (Norton XZ16052) onto the wafer. Theslurry was composed of 1.5 g zirconia powder in 4 mL of a MEO/EG/H₂O40:30:30 mixture. A total of 3 μL of slurry was deposited on each spot.

[0255] The zirconia carrier precoated wafer was impregnated with 7Pconcentration gradients of Ti, Zr, V, Mo and Co and 8P concentrationgradients of Ge, Sn, Sb, La and Ce by Cavro dispensing from metal stocksolutions vials to a microtiter plate followed by transferring replicasof the gradients onto the wafer (2.5 μl dispense volume per well). Co,La and Ce were provided as their nitrates, Zr as the zirconyl nitrate,Ti as the ammonium titanyl oxalate, Sb as ammonium antimony oxalate, V,Ge and Sn as their oxalates and Mo as molybdic acid. The wafer was driedat 70° C. for 10 minutes and then a 7 and 8 point gradients of Fe, Ruand Rh were transferred from a microtiter plate to the wafer (2.5 μldispense volume/well.) Fe and Rh were provided as their nitrates, Ru asthe nitrosyl nitrate. The wafer was dried at 70° C. for 10 minutes andthen was uniformly coated with 2.5 μl/well of a Pt(NH₃)₂(NO₂)₂ stocksolution (1% Pt).

[0256] The wafer was dried at 70° C. for 10 minutes, calcined in air at450° C. for 2 hours, then reduced in 5% H₂/Ar at 450° C. for 2 hours.Nine internal standards were synthesized by spotting 2.5 μlPt(NH₃)₂(NO₂)₂ solution (1.0% Pt) into the corresponding first row/lastcolumn positions. See FIGS. 10A through 10F.

[0257] The reduced library was then screened in SMS for WGS activitywith a H₂/CO/CO₂/H₂O mixed feed at 300° C. and 350° C. The CO conversionversus CO₂ production results at 300° C. and 350° C. are presented inFIGS. 10G, 10H and 101. More detailed test results, such as, COconversion, CO₂ production and CH₄ production at 250° C. and 300° C. foreach of the 225 individual catalyst wells on the test wafer arepresented in Table 4.

[0258] This set of experiments demonstrated active and selective WGScatalyst formulations of Pt—Ru—{Ti, Zr, V, Mo, Co, Ge, Sn, Sb, La, Ce}compositions on the wafer.

Example 11

[0259] A 4″ quartz wafer was precoated with zirconia carrier by repeatedslurry dispensing zirconia powder (Norton XZ16052) onto the wafer. Theslurry was composed of 1.5 g zirconia powder in 4 mL of a MEO/EG/H₂O40:30:30 mixture. A total of 3 μL of slurry was deposited on each spot.

[0260] The zirconia carrier precoated wafer was impregnated with 5Pconcentration gradients of Co, Ru and Mo by Cavro dispensing from metalstock solutions vials to a microtiter plate followed by transferringreplicas of the gradients onto the wafer (2.5 μl dispense volume perwell). Co was provided as its nitrate, Mo as molybdic acid and Ru as thenitrosyl nitrate. The wafer was dried at 70° C. for 10 minutes.

[0261] The wafer was then impregnated with 5P concentration gradients ofCe, Co, Ru, La, Zr, Cu, Re and Ge. Ce was provided as its nitrate and asammonium cerium(IV) nitrate; Co as its acetate and as sodiumhexanitrocobaltate(III); Ru as potassium perruthenate, KRuO₄, rutheniumnitrosyl acetate, Ru(NO)(OAc)₃; La and Cu as their nitrates; Zr aszirconyl nitrate and zirconyl acetate; Re as NH₄ReO₄; and Ge as theoxalate.

[0262] The wafer was dried at 70° C. for 10 minutes and then wasuniformly coated with 2.5 μl/well of a Pt(NH₃)₂(NO₂)₂ stock solution (1%Pt).

[0263] The wafer was dried at 70° C. for 10 minutes, calcined in air at350° C. for 2 hours, then reduced in 5% H₂/Ar at 300° C. for 2 hours.Nine internal standards were synthesized by spotting 2.5 μlPt(NH₃)₂(NO₂)₂ solution (1.0% Pt) into the corresponding first row/lastcolumn positions. See FIGS. 11A through 11F.

[0264] The reduced library was then screened in SMS for WGS activitywith a H₂₁CO/CO₂/H₂O mixed feed at 250° C. The CO conversion versus CO₂production results at 250° C. are presented in FIG. 11G. More detailedtest results, such as, CO conversion, CO₂ production and CH₄ productionat 250° C. for each of the 225 individual catalyst wells on the testwafer are presented in Table 5.

[0265] This set of experiments demonstrated active and selective WGScatalyst formulations of Pt—Ru—{Co, Ce, Mo, Na, K, La, Zr, Re, Cu, Ge}compositions on the wafer.

Example 12

[0266] Scale-up catalyst samples were prepared by using incipientwetness impregnation of 2.5 grams of ZrO₂ support (Norton, 80-120 mesh)which had been weighed into a 10-dram vial. Aqueous metal precursor saltsolutions were then added in the order Ru, Co, Pt and Na. The precursorsalt solutions are set forth in Table 7. Following each metal addition,the catalysts were dried at 80° C. overnight and then calcined in air asfollows:

[0267] After Ru or Co addition—450° C. for 3 hours

[0268] After Pt addition—300° C. for 3 hours.

[0269] Following Na addition, the catalysts were calcined at 300° C. for3 hours, and then the catalysts were reduced in-situ at 300° C. for 3hours in a 10% H₂/N₂ feed. TABLE 6 Catalyst compositions Catalyst ID %Ru % Co % Pt % Na 1001-01 0.5 0.5 6 5 1001-02 0.5 1 6 5 1001-03 0.5 1.56 5 1001-04 1 0.5 6 5 1001-05 1 1 6 5 1001-06 1 1.5 6 5 1001-07 1.5 0.56 5 1001-08 1.5 1 6 5 1001-09 1.5 1.5 6 5 1001-10 1 1 6 0 1001-11 1 1 35 1001-12 1 1 6 7.5 1001-13 0 1 6 0 1001-14 0 1 6 5

[0270] TABLE 7 Metal precursors Precursor Concentration Ru(NO)(NO₃)₃1.5% Ru w/w Co(NO₃)₂ 1 Molar Pt(NH₃)₄(OH)₂ 9.06% Pt w/w NaOH 3 Molar

[0271] Catalyst Testing Conditions

[0272] Catalysts were tested in a fixed bed reactor. Approximately 0.15g of catalyst was weighed and mixed with an equivalent mass of SiC. Themixture was loaded into a reactor and heated to reaction temperature.Reaction gases were delivered via mass flow controllers (Brooks) withwater introduced with a metering pump (Quizix). The composition of thereaction mixture was as follows: H₂ 50%, CO 10%, CO₂ 10%, and H₂O 30%.The reactant mixture was passed through a pre-heater before contactingthe catalyst bed. Following reaction, the product gases were analyzedusing a micro gas chromatograph (Varian). Compositional data on thespace velocity diagrams are on a dry basis with water removed.

[0273] Testing Results

[0274]FIGS. 12A through 12C show the CO composition in the productstream following the scale-up testing at gas hour space velocities of50,000, 100,000 and 150,000 h⁻¹. All materials showed WGS activity atthe tested temperatures and space velocities as shown. Selectivies wereall greater than 99% to CO₂ with the exception of catalyst sample 1001-8(selectivity of 98.5% to CO₂ at GHSV=50,000 at 325° C.).

Example 13

[0275] Scale-up catalyst samples were prepared by using incipientwetness impregnation of 0.75 grams of ZrO₂ support (Norton, 80-120 mesh)which had been weighed into a 10-dram vial. Aqueous metal precursor saltsolutions were then added in the order Ru, Pt and one of Na, K, or Li.The precursor salt solutions were tetraammineplatinum (II) hydroxide(9.09% Pt (w/w)), ruthenium (III) nitrosylnitrate (1.5% Ru (w/v)),sodium hydroxide (3.0N), lithium hydroxide monohydrate (2.5M), andpotassium hydroxide (13.92% K). All reagents were nominally researchgrade from Aldrich, Strem, or Alfa. Following each metal addition, thecatalysts were dried at 80° C. overnight and then calcined in air asfollows:

[0276] After Ru addition—450° C. for 3 hours

[0277] After Pt addition—300° C. for 3 hours

[0278] Following Na, K, or Li addition, the catalysts were calcined at300° C. for 3 hours, and then the catalysts were reduced in-situ at 300°C. for 3 hours in a 10% H₂/N₂ feed.

[0279] Catalyst Testing Conditions

[0280] Catalysts were tested in a fixed bed reactor. Approximately 0.15g of catalyst was weighed and mixed with an equivalent mass of SiC. Themixture was loaded into a reactor and heated to reaction temperature.Reaction gases were delivered via mass flow controllers (Brooks) withwater introduced with a metering pump (Quizix). The composition of thereaction mixture was as follows: H₂ 50%, CO 10%, CO₂ 10%, and H₂O 30%.The reactant mixture was passed through a pre-heater before contactingthe catalyst bed. Following reaction, the product gases were analyzedusing a micro gas chromatograph (Varian Instruments, or Shimadzu).Compositional data on the performance diagram (FIG. 13) is on a drybasis with water removed.

[0281] Testing Results

[0282]FIG. 13 shows the CO composition in the product stream followingthe scale-up testing at gas hour space velocities of 50,000 h⁻¹. TABLE 8Catalyst Composition (mass ratio) Row Col Support Ru Pt Na K Li A 10.905 0.01 0.06 0.025 0 0 A 2 0.88 0.01 0.06 0.05 0 0 A 3 0.905 0.010.06 0 0.025 0 A 4 0.88 0.01 0.06 0 0.05 0 A 5 0.905 0.01 0.06 0 0 0.025A 6 0.88 0.01 0.06 0 0 0.05 B 1 0.905 0.01 0.06 0.025 0 0 B 2 0.88 0.010.06 0.05 0 0 B 3 0.905 0.01 0.06 0 0.025 0 B 4 0.88 0.01 0.06 0 0.05 0B 5 0.905 0.01 0.06 0 0 0.025 B 6 0.88 0.01 0.06 0 0 0.05 C 1 0.895 0.020.06 0.025 0 0 C 2 0.87 0.02 0.06 0.05 0 0 C 3 0.895 0.02 0.06 0 0.025 0C 4 0.87 0.02 0.06 0 0.05 0 C 5 0.895 0.02 0.06 0 0 0.025 C 6 0.87 0.020.06 0 0 0.05 D 1 0.895 0.02 0.06 0.025 0 0 D 2 0.87 0.02 0.06 0.05 0 0D 3 0.895 0.02 0.06 0 0.025 0 D 4 0.87 0.02 0.06 0 0.05 0 D 5 0.895 0.020.06 0 0 0.025 D 6 0.87 0.02 0.06 0 0 0.05

Example 14

[0283] Scale-up catalyst samples were prepared by using incipientwetness impregnation of 0.75 grams of ZrO₂ support (Norton, 80-120 mesh)which had been weighed into a 10-dram vial. Aqueous metal precursor saltsolutions were then added in the order: Ru, one of Y, Sc, or La, and Pt.The precursor salt solutions were tetraammineplatimum (II) hydroxide(9.09% Pt (w/w)), ruthenium (III) nitrosylnitrate (1.5% Ru), yttrium(III) nitrate (1.0M), scandium (III) nitrate (4.2% Sc), lanthanum (III)nitrate (1.0M), and potassium hydroxide (13.92% K). All reagents werenominally research grade from Aldrich, Strem, or Alfa. Following eachmetal addition, the catalysts were dried at 80° C. overnight and thencalcined in air-as follows: After Ru addition 450° C. for 3 hours AfterPt addition 300° C. for 3 hours After Y, Sc, or La addition 450° C. for3 hours.

[0284] Following the final addition, the catalysts were reduced in-situat 300° C. for 3 hours in a 10% H₂/N₂ feed.

[0285] Catalyst Testing Conditions

[0286] Catalysts were tested in a fixed bed reactor. Approximately 0.15g of catalyst was weighed and mixed with an equivalent mass of SiC. Themixture was loaded into a reactor and heated to reaction temperature.Reaction gases were delivered via mass flow controllers (Brooks) withwater introduced with a metering pump (Quizix). The composition of thereaction mixture was as follows: H₂ 50%, CO 10%, CO₂ 10%, and H₂O 30%.The reactant mixture was passed through a pre-heater before contactingthe catalyst bed. Following reaction, the product gases were analyzedusing a micro gas chromatograph (Varian Instruments, or Shimadzu).Compositional data on the performance diagram (FIG. 14) is on a drybasis with water removed.

[0287] Testing Results

[0288]FIG. 14 shows the CO composition in the product stream followingthe scale-up testing at gas hour space velocities of 50,000 h⁻¹. TABLE 9Catalyst Composition (mass ratio) Row Col Support Ru Pt Y Sc La A 10.905 0.01 0.06 0.025 0 0 A 2 0.88 0.01 0.06 0.05 0 0 A 3 0.905 0.010.06 0 0.025 0 A 4 0.88 0.01 0.06 0 0.05 0 A 5 0.905 0.01 0.06 0 0 0.025A 6 0.88 0.01 0.06 0 0 0.05 B 1 0.905 0.01 0.06 0.025 0 0 B 2 0.88 0.010.06 0.05 0 0 B 3 0.905 0.01 0.06 0 0.025 0 B 4 0.88 0.01 0.06 0 0.05 0B 5 0.905 0.01 0.06 0 0 0.025 B 6 0.88 0.01 0.06 0 0 0.05 C 1 0.895 0.020.06 0.025 0 0 C 2 0.87 0.02 0.06 0.05 0 0 C 3 0.895 0.02 0.06 0 0.025 0C 4 0.87 0.02 0.06 0 0.05 0 C 5 0.895 0.02 0.06 0 0 0.025 C 6 0.87 0.020.06 0 0 0.05 D 1 0.895 0.02 0.06 0.025 0 0 D 2 0.87 0.02 0.06 0.05 0 0D 3 0.895 0.02 0.06 0 0.025 0 D 4 0.87 0.02 0.06 0 0.05 0 D 5 0.895 0.020.06 0 0 0.025 D 6 0.87 0.02 0.06 0 0 0.05

Example 15

[0289] Scale-up catalyst samples were prepared by using incipientwetness impregnation of 0.75 grams of ZrO₂ support (Norton, 80-120 mesh)which had been weighed into a 10-dram vial. Aqueous metal precursor saltsolutions were then added in the order: Ru, V, Pt, and finally Na. Theprecursor salt solutions were tetraammineplatinum (II) hydroxidesolution (9.09% Pt (w/w)), ruthenium (III) nitrosylnitrate (1.5% Ru(w/v), vanadium citrate (1.0M), and sodium hydroxide (3.0 N). Allstarting reagents were nominally research grade from Aldrich, Strem, orAlfa. Following each metal addition, the catalysts were dried at 80° C.overnight and then calcined in air as follows: After Pt addition 300° C.for 3 hours After Ru addition 450° C. for 3 hours After V addition 350°C. for 3 hours.

[0290] Following Na addition, the catalysts were calcined at 300° C. for3 hours, and then the catalysts were reduced in-situ at 300° C. for 3hours in a 10% H₂/N₂ feed.

[0291] Catalyst Testing Conditions

[0292] Catalysts were tested in a fixed bed reactor. Approximately 0.15g of catalyst was weighed and mixed with an equivalent mass of SiC. Themixture was loaded into a reactor and heated to reaction temperature.Reaction gases were delivered via mass flow controllers (Brooks) withwater introduced with a metering pump (Quizix). The composition of thereaction mixture was as follows: H₂ 50%, CO 10%, CO₂ 10%, and H₂O 30%.The reactant mixture was passed through a pre-heater before contactingthe catalyst bed. Following reaction, the product gases were analyzedusing a micro gas chromatograph (Varian Instruments, or Shimadzu).Compositional data on the performance diagram (FIG. 17) is on a drybasis with water removed.

[0293] Testing Results

[0294]FIG. 17 shows the CO composition in the product stream followingthe scale-up testing at a gas hour space velocity of 50,000 h⁻¹. TABLE10 Catalyst Compositions (mass ratio) Cat ID Support Pt Ru V Na 1006−0191.03 6.00 0.25 0.22 2.50 1006−02 90.81 6.00 0.25 0.43 2.50 1006−0390.37 6.01 0.25 0.87 2.50 1006−04 88.53 6.00 0.25 0.22 5.00 1006−0588.31 6.00 0.25 0.43 5.00 1006−06 87.87 6.01 0.25 0.87 5.01 1006−0786.03 6.00 0.25 0.22 7.50 1006−08 85.81 6.00 0.25 0.43 7.51 1006−0985.37 6.01 0.25 0.87 7.51 1006−10 90.78 6.00 0.50 0.22 2.50 1006−1188.28 6.00 0.50 0.22 5.00 1006−12 85.78 6.00 0.50 0.22 7.50

[0295] TABLE I Tem- pera- ture: 250 C. Pt1.0%/ R C COCONV H2OCONVCO2PROD CO2PERPROD CH4PROD Zr 02_std LaNO33 real real real real realreal real real real 1 1 24.0554 20.3567 1.0059 36.8713 0.1785 0.1275 0 12 −1.7201 3.3539 0.049 1.7972 0.0067 0 0 1 3 −1.3278 2.2499 0.00090.0315 −0.0026 0 0 1 4 −1.208 2.4958 0.005 0.1823 −0.0038 0 0 1 5−1.3966 −0.6647 0.0138 0.5067 −0.0024 0 0 1 6 −0.857 −0.806 0.00890.3249 −0.0058 0 0 1 7 26.8747 16.7142 0.9416 34.513 0.151 0.1275 0 1 8−0.1762 0.0001 0.0106 0.3868 −0.0076 0 0 1 9 −0.605 −1.4054 0.00160.0598 −0.0081 0 0 1 10 −0.1705 5.1803 −0.0005 −0.0171 −0.0108 0 0 1 110.0287 −2.3403 −0.0261 −0.9568 −0.0134 0 0 1 12 −0.3619 −2.3753 −0.0191−0.6997 −0.0107 0 0 1 13 26.9134 15.6985 0.9206 33.7449 0.1456 0.1275 01 14 0.2866 −1.4436 0.0104 0.3794 −0.0009 0 0 1 15 −0.2691 −2.5021−0.0098 −0.3592 −0.0125 0 0 1 16 26.3015 15.0776 0.9071 33.2485 0.14220.1275 0 2 1 10.3797 7.5635 0.2714 9.9469 0.0465 0 0 2 2 22.2742 13.62560.7038 25.7961 0.1014 0 0 2 3 20.1518 11.8043 0.6181 22.6557 0.0925 0 02 4 14.7068 7.5278 0.4396 16.1127 0.074 0 0 2 5 12.5748 6.9812 0.353812.9691 0.0619 0 0 2 6 12.5733 7.5902 0.3721 13.6375 0.065 0 0 2 73.9682 1.1157 0.1053 3.861 0.0291 0 0 2 8 4.2902 1.5276 0.1017 3.7280.0316 0 0 2 9 17.5859 9.8527 0.5611 20.5685 0.0868 0 0 2 10 4.00560.7967 0.1073 3.9343 0.0337 0 0 2 11 0.4511 −1.4852 −0.0262 −0.96110.0142 0 0 2 12 8.7515 3.1358 0.2704 9.9096 0.0534 0 0 2 13 1.1667−0.4291 0.0028 0.1022 0.0172 0 0 2 14 5.3788 3.039 0.1661 6.0891 0.04020 0 2 15 13.8175 7.9862 0.4538 16.6329 0.0753 0 0.625 2 16 0.5892 0.0397−0.0171 −0.6274 −0.0021 0 0 3 1 23.0341 14.9411 0.7335 26.8867 0.1082 00 3 2 24.8268 16.0912 0.7611 27.8973 0.108 0 0 3 3 21.0312 12.21630.6617 24.2545 0.0974 0 0 3 4 15.3062 8.5994 0.4563 16.7247 0.0714 0 0 35 13.1818 6.4699 0.3775 13.8381 0.0651 0 0 3 6 14.4778 9.2713 0.424115.5437 0.0643 0 0 3 7 5.5717 3.3425 0.1029 3.772 0.0251 0 0 3 8 6.82281.6923 0.1521 5.5733 0.0283 0 0 3 9 18.2423 12.1678 0.5606 20.54680.0831 0 0 3 10 6.7011 5.5857 0.1612 5.907 0.033 0 0 3 11 1.3529 1.3312−0.0328 −1.2024 0.0065 0 0 3 12 8.988 6.9454 0.2544 9.3233 0.0421 0 0 313 1.9882 1.6201 −0.0124 −0.4561 0.0102 0 0 3 14 6.7207 4.8802 0.12834.7036 0.0288 0 0 3 15 13.1254 7.8413 0.4144 15.1912 0.0623 0 0.625 3 161.6968 −0.6116 −0.0065 −0.238 0.007 0 0 4 1 25.6701 19.5197 0.751427.5411 0.0986 0 0 4 2 23.653 16.9227 0.7928 29.0607 0.0984 0 0 4 322.8118 16.1844 0.6593 24.168 0.0919 0 0 4 4 16.4182 10.7873 0.483717.731 0.0754 0 0 4 5 14.5564 7.5137 0.4146 15.1965 0.0579 0 0 4 515.7933 9.8273 0.453 16.6027 0.0657 0 0 4 7 6.1716 5.3192 0.1362 4.99350.0244 0 0 4 8 7.1386 3.6867 0.1822 6.6787 0.0338 0 0 4 9 20.730313.3734 0.6248 22.9033 0.0886 0 0 4 10 8.9131 3.194 0.1982 7.2642 0.03340 0 4 11 1.6189 1.2404 −0.0525 −1.926 −0.0002 0 0 4 12 10.7432 5.7820.2838 10.4022 0.045 0 0 4 13 1.5884 0.8166 −0.0105 −0.3833 0.0101 0 0 414 6.4031 3.2336 0.1734 6.3554 0.0362 0 0 4 15 15.6125 10.3811 0.471317.2763 0.0703 0 0.625 4 16 27.9195 15.9998 0.8541 31.3081 0.1277 0.12750 5 1 23.5648 16.7387 0.7605 27.8743 0.1008 0 0 5 2 24.3053 17.34860.7802 28.5962 0.1046 0 0 5 3 22.341 15.7024 0.7107 26.0515 0.1019 0 0 54 17.6158 11.8733 0.5469 20.0479 0.0791 0 0 5 5 14.2387 10.1452 0.404914.8406 0.0574 0 0 5 6 15.1152 10.7747 0.4328 15.8622 0.0615 0 0 5 76.2094 5.1538 0.1363 4.9969 0.0249 0 0 5 8 7.6993 4.4249 0.2079 7.61920.0348 0 0 5 9 20.3032 12.9878 0.6687 24.5092 0.091 0 0 5 10 10.4677.0359 0.2642 9.6824 0.0427 0 0 5 11 2.8488 0.9928 −0.0496 −1.8191−0.0034 0 0 5 12 8.6081 4.7427 0.2975 10.9032 0.0379 0 0 5 13 2.47860.2441 −0.0353 −1.2925 0.0105 0 0 5 14 5.1083 3.0311 0.1416 5.192 0.02850 0 5 15 11.8585 7.5495 0.3716 13.62 0.0576 0 0.625 5 16 0.172 0.0674−0.0092 −0.3389 0.01 0 0 6 1 22.8548 15.2481 0.7655 28.0601 0.1096 0 0 62 25.4205 16.425 0.8006 29.3446 0.11 0 0 6 3 25.0359 16.7118 0.774228.379 0.1081 0 0 6 4 19.8242 13.56 0.6037 22.1285 0.0864 0 0 6 515.5667 10.9252 0.4506 16.5181 0.0668 0 0 6 6 14.9248 9.1668 0.484817.7684 0.0716 0 0 6 7 6.2748 4.0969 0.1824 6.6868 0.0317 0 0 6 8 8.48585.8883 0.251 9.2019 0.0404 0 0 6 9 21.0027 12.7923 0.7581 27.7862 0.10150 0 6 10 4.1864 1.0991 0.2231 8.177 0.044 0 0 6 11 −1.2373 −1.43930.0135 0.4931 0.0092 0 0 5 12 10.6286 6.8786 0.3149 11.5433 0.0492 0 0 613 1.0716 0.1767 0.0081 0.2959 0.0131 0 0 6 14 6.6959 4.4786 0.17426.3849 0.0291 0 0 6 15 14.9263 8.9373 0.4504 16.5076 0.0691 0 0.625 6 160.9734 0.524 −0.0068 −0.2476 0.0095 0 0 7 1 22.5418 15.4759 0.72626.6121 0.0978 0 0 7 2 25.3352 17.1813 0.8109 29.7233 0.1123 0 0 7 325.4575 17.3091 0.7912 29.0012 0.1094 0 0 7 4 20.6572 14.3391 0.631323.1392 0.0896 0 0 7 5 15.932 11.3449 0.4504 16.51 0.0654 0 0 7 615.7862 11.3444 0.4701 17.2316 0.0672 0 0 7 7 6.5518 5.4328 0.16095.8983 0.0264 0 0 7 8 8.798 5.7477 0.2274 8.3369 0.0394 0 0 7 9 23.007515.3925 0.6659 24.4074 0.0863 0 0 7 10 9.2334 7.3996 0.2983 10.9340.0356 0 0 7 11 0.7033 0.897 −0.0323 −1.1825 0.0007 0 0 7 12 9.88126.9932 0.3106 11.3832 0.047 0 0 7 13 1.8315 1.5281 −0.0004 −0.01420.0064 0 0 7 14 5.9233 4.0164 0.1346 4.9347 0.024 0 0 7 15 11.39817.0352 0.3499 12.8255 0.0508 0 0.625 7 16 26.5669 16.7815 0.8474 31.06240.1182 0.1275 0 8 1 22.7201 15.0948 0.694 25.4388 0.0942 0 0 8 2 25.596816.5345 0.8165 29.9286 0.1106 0 0 8 3 26.9015 16.5093 0.8118 29.75560.1132 0 0 8 4 22.6912 14.399 0.6735 24.6849 0.0922 0 0 8 5 16.151310.0868 0.4873 17.8622 0.0711 0 0 8 6 14.9604 9.3549 0.5104 18.70930.0788 0 0 8 7 9.1106 4.8845 0.1351 4.9537 0.0227 0 0 8 8 11.6445 4.27590.265 9.7129 0.0431 0 0 8 9 22.1496 13.0101 0.7517 27.5537 0.103 0 0 810 10.7574 7.0805 0.323 11.8395 0.0477 0 0 8 11 3.6004 0.9577 0.03831.4029 0.0094 0 0 8 12 11.534 7.8883 0.3533 12.9484 0.0508 0 0 8 131.3464 0.5169 −0.0012 −0.0457 0.0054 0 0 8 14 6.4094 3.371 0.1695 6.21440.0276 0 0 8 15 12.8137 8.3353 0.3838 14.067 0.054 0 0.625 8 16 0.60050.7618 −0.0245 −0.8983 0.0023 0 0 9 1 22.4957 14.7378 0.6826 25.01930.0926 0 0 9 2 25.986 17.2218 0.8042 29.4787 0.1075 0 0 9 3 26.727817.0659 0.8299 30.4191 0.1155 0 0 9 4 21.7825 14.3953 0.6911 25.33060.0965 0 0 9 5 17.2508 11.3087 0.5012 18.3711 0.0717 0 0 9 6 16.958110.5872 0.4639 17.0022 0.0651 0 0 9 7 6.3335 4.0566 0.1665 6.1027 0.03260 0 9 8 11.9448 6.8015 0.2794 10.2426 0.0347 0 0 9 9 22.3682 14.30680.6953 25.4874 0.0927 0 0 9 10 10.6395 6.5727 0.3015 11.0498 0.0426 0 09 11 0.7463 −0.5268 −0.0297 −1.0885 0.0037 0 0 9 12 11.6436 6.90320.3308 12.1271 0.0465 0 0 9 13 2.2734 1.3731 −0.0036 −0.1307 0.0063 0 09 14 5.2473 2.3383 0.133 4.8766 0.0256 0 0 9 15 14.1744 8.1484 0.438616.0753 0.0629 0 0.625 9 16 1.1167 0.6406 −0.0074 −0.2708 0.0074 0 0 101 21.0706 14.7112 0.6846 25.0928 0.0968 0 0 10 2 26.8869 17.9825 0.885932.4724 0.1184 0 0 10 3 26.6813 16.9521 0.9023 33.0744 0.1263 0 0 10 422.8526 14.0275 0.7543 27.65 0.106 0 0 10 5 16.4643 9.638 0.5121 18.7720.0768 0 0 10 6 16.974 10.2305 0.4989 18.2853 0.0738 0 0 10 7 7.07643.7892 0.217 7.954 0.0367 0 0 10 8 10.3301 7.0156 0.3079 11.2846 0.04440 0 10 9 22.9265 14.8712 0.7519 27.5603 0.1024 0 0 10 10 12.4677 6.99630.3574 13.1014 0.0529 0 0 10 11 0.5969 −0.5299 −0.0215 −0.7876 0.0033 00 10 12 13.3324 8.0107 0.3981 14.593 0.0579 0 0 10 13 1.9031 0.56980.0129 0.4715 0.0076 0 0 10 14 6.4847 3.7801 0.156 5.7172 0.0292 0 0 1015 13.3979 8.7146 0.4385 16.0738 0.0621 0 0.625 10 16 25.4495 16.04770.8342 30.5766 0.1176 0.1275 0 11 1 20.1375 13.3902 0.695 25.4752 0.09410 0 11 2 27.139 17.1786 0.8841 32.4048 0.1236 0 0 11 3 26.9388 16.6830.9125 33.4483 0.127 0 0 11 4 24.5762 15.8875 0.789 28.9207 0.1089 0 011 5 15.1923 9.882 0.4773 17.4944 0.0718 0 0 11 6 15.7362 10.517 0.495918.1782 0.0704 0 0 11 7 6.9524 4.547 0.2149 7.8771 0.0338 0 0 11 810.7228 5.8543 0.3063 11.2265 0.0473 0 0 11 9 21.6871 13.7234 0.738127.0563 0.1017 0 0 11 10 10.2552 6.749 0.3273 11.9961 0.0462 0 0 11 110.1751 −0.8137 −0.0162 −0.5948 0.0093 0 0 11 12 12.9233 7.3461 0.395914.5118 0.058 0 0 11 13 2.1161 −0.0461 0.0196 0.7173 0.0121 0 0 11 145.318 2.5839 0.1421 5.2076 0.028 0 0 11 15 12.7569 6.3017 0.3941 14.44560.0579 0 0.625 11 16 0.8455 −1.3583 0.0027 0.0985 0.0084 0 0 12 115.9884 10.3576 0.5209 19.0939 0.0763 0 0 12 2 27.3984 16.7714 0.924133.8719 0.128 0 0 12 3 28.1625 17.4315 0.9325 34.1804 0.1313 0 0 12 424.8213 15.2594 0.851 31.1941 0.1246 0 0 12 5 16.5105 9.4519 0.571520.9463 0.089 0 0 12 6 16.2367 8.6629 0.5246 19.229 0.0791 0 0 12 77.0822 2.7268 0.2494 9.143 0.0433 0 0 12 8 11.1025 6.1665 0.3763 13.79410.056 0 0 12 9 23.5429 14.4559 0.8026 29.419 0.1129 0 0 12 10 12.41697.2141 0.384 14.0754 0.0576 0 0 12 11 −0.2192 −1.5288 −0.0114 −0.41950.0063 0 0 12 12 13.2567 7.0496 0.4182 15.3281 0.0611 0 0 12 13 1.2187−0.6308 0.0286 1.0496 0.0116 0 0 12 14 5.5276 1.9229 0.1649 6.04260.0328 0 0 12 15 13.3469 6.2659 0.4232 15.5137 0.0634 0 0.625 12 161.0083 −0.586 0.011 0.4039 0.0096 0 0 13 1 18.6644 11.2964 0.650623.8458 0.0932 0 0 13 2 27.845 15.9413 0.9392 34.4261 0.1308 0 0 13 327.3697 17.3186 0.9442 34.6097 0.1337 0 0 13 4 25.678 15.9207 0.840130.7915 0.1183 0 0 13 5 15.7945 10.0005 0.5228 19.164 0.0793 0 0 13 615.3463 9.2398 0.5087 18.6471 0.0765 0 0 13 7 6.7754 3.6609 0.2308 8.4590.0396 0 0 13 8 11.692 6.4553 0.3752 13.7513 0.0561 0 0 13 9 23.280913.521 0.8112 29.7353 0.1124 0 0 13 10 13.5562 7.5286 0.4302 15.76760.0624 0 0 13 11 1.1357 −1.0497 −0.0258 −0.9457 0.0072 0 0 13 12 14.08927.0847 0.4404 16.1411 0.0683 0 0 13 13 1.2307 −0.0972 0.0411 1.50480.0161 0 0 13 14 5.0473 1.1814 0.1519 5.5685 0.0306 0 0 13 15 12.88946.9657 0.3932 14.413 0.0574 0 0.625 13 16 27.0196 15.8321 0.9126 33.4490.1349 0.1275 0 14 1 21.6824 14.5808 0.7642 28.0108 0.1054 0 0 14 227.9534 18.5673 0.9122 33.4357 0.1269 0 0 14 3 28.3871 17.6025 0.950634.8433 0.1361 0 0 14 4 26.5322 15.1329 0.8627 31.6204 0.1283 0 0 14 517.27 10.4633 0.5486 20.1091 0.0846 0 0 14 6 16.6826 9.6418 0.572120.9704 0.0848 0 0 14 7 7.7667 4.5307 0.2694 9.8752 0.0433 0 0 14 813.2575 8.5866 0.4374 16.0317 0.064 0 0 14 9 24.5972 16.2327 0.825530.2566 0.1118 0 0 14 10 14.1237 8.1483 0.478 17.5191 0.0713 0 0 14 11−0.172 −1.5106 −0.0204 −0.7482 0.0089 0 0 14 12 15.8277 8.9664 0.507618.6043 0.0706 0 0 14 13 1.0637 −1.0104 0.0444 1.6268 0.0139 0 0 14 144.6635 2.3532 0.1677 6.1462 0.0296 0 0 14 15 12.9488 7.3298 0.429615.7453 0.0651 0 0.625 14 16 0.3061 −0.5069 −0.0065 −0.2391 0.0099 0 015 1 17.1998 12.0104 0.5755 21.0955 0.0799 0 0 15 2 27.4482 17.526 0.93334.1967 0.1316 0 0 15 3 28.1178 18.8556 0.9242 33.8763 0.1324 0 0 15 426.8701 17.1463 0.856 31.3778 0.1258 0 0 15 5 17.6631 10.9667 0.584521.4248 0.0858 0 0 15 6 17.1402 10.8854 0.5425 19.8853 0.0798 0 0 15 78.2663 5.3027 0.2441 8.9487 0.0387 0 0 15 8 11.9892 6.7241 0.390414.3081 0.0566 0 0 15 9 24.1606 15.639 0.8291 30.3902 0.1118 0 0 15 1015.0377 10.3936 0.4614 16.9136 0.0638 0 0 15 11 0.2191 −0.9933 −0.0152−0.558 0.0074 0 0 15 12 16.1138 9.1228 0.5094 18.6707 0.0732 0 0 15 132.4821 0.3422 0.0309 1.1317 0.0144 0 0 15 14 5.4454 0.6463 0.189 6.92760.035 0 0 15 15 14.0229 7.8558 0.4492 16.4654 0.0681 0 0.625 15 160.4686 −0.7131 0.0197 0.7216 0.01 0 0 16 1 7.4861 4.4402 0.2493 9.13860.0401 0 0 16 2 29.0506 17.8613 0.9483 34.7579 0.1412 0 0 16 3 29.469417.4993 0.9236 33.8554 0.1479 0 0 16 4 28.4749 16.4322 0.9104 33.36930.1531 0 0 16 5 22.0326 12.6858 0.7055 25.8606 0.1115 0 0 16 6 20.080512.1402 0.6291 23.0594 0.0943 0 0 16 7 9.0587 5.2161 0.2666 9.77030.0461 0 0 16 8 13.983 9.3075 0.4391 16.0948 0.0636 0 0 16 9 26.990517.0719 0.877 32.1456 0.1198 0 0 16 10 14.704 8.6762 0.4886 17.91020.073 0 0 16 11 0.7191 −1.4742 −0.0041 −0.1519 0.0077 0 0 16 12 19.31411.1355 0.6495 23.808 0.0899 0 0 16 13 2.4636 0.033 0.0679 2.4886 0.02060 0 16 14 11.4461 6.8975 0.3856 14.134 0.0639 0 0 16 15 20.8264 13.16230.7 25.6595 0.0961 0 0.625 16 16 26.7851 15.9945 0.9048 33.1661 0.13190.1275 0 Tem- pera- ture: 250 C. SUM_(—) mol % mol % mol % R CPtNH32NO22 ZrONO32 micromols La Pt Zr real real real real 1 1 0 0 0.12750 100 0 1 2 0 0 0 0 0 0 1 3 0 0 0 0 0 0 1 4 0 0 0 0 0 0 1 5 0 0 0 0 0 01 6 0 0 0 0 0 0 1 7 0 0 0.1275 0 100 0 1 8 0 0 0 0 0 0 1 9 0 0 0 0 0 0 110 0 0 0 0 0 0 1 11 0 0 0 0 0 0 1 12 0 0 0 0 0 0 1 13 0 0 0.1275 0 100 01 14 0 0 0 0 0 0 1 15 0 0 0 0 0 0 1 16 0 0 0.1275 0 100 0 2 1 0.0319 00.0319 0 100 0 2 2 0.0319 0 0.0319 0 100 0 2 3 0.0319 0 0.0319 0 100 0 24 0.0319 0 0.0319 0 100 0 2 5 0.0319 0 0.0319 0 100 0 2 6 0.0319 00.0319 0 100 0 2 7 0.0319 0 0.0319 0 100 0 2 8 0.0319 0 0.0319 0 100 0 29 0.0319 0 0.0319 0 100 0 2 10 0.0319 0 0.0319 0 100 0 2 11 0.0319 00.0319 0 100 0 2 12 0.0319 0 0.0319 0 100 0 2 13 0.0319 0 0.0319 0 100 02 14 0.0319 0.625 0.6569 0 4.85 95.15 2 15 0.0319 0 0.6569 95.15 4.85 02 16 0 0 0 0 0 0 3 1 0.0387 0 0.0387 0 100 0 3 2 0.0387 0 0.0387 0 100 03 3 0.0387 0 0.0387 0 100 0 3 4 0.0387 0 0.0387 0 100 0 3 5 0.0387 00.0387 0 100 0 3 6 0.0387 0 0.0387 0 100 0 3 7 0.0387 0 0.0387 0 100 0 38 0.0387 0 0.0387 0 100 0 3 9 0.0387 0 0.0387 0 100 0 3 10 0.0387 00.0387 0 100 0 3 11 0.0387 0 0.0387 0 100 0 3 12 0.0387 0 0.0387 0 100 03 13 0.0387 0 0.0387 0 100 0 3 14 0.0387 0.625 0.6637 0 5.83 94.17 3 150.0387 0 0.6637 94.17 5.83 0 3 16 0 0 0 0 0 0 4 1 0.0455 0 0.0455 0 1000 4 2 0.0455 0 0.0455 0 100 0 4 3 0.0455 0 0.0455 0 100 0 4 4 0.0455 00.0455 0 100 0 4 5 0.0455 0 0.0455 0 100 0 4 5 0.0455 0 0.0455 0 100 0 47 0.0455 0 0.0455 0 100 0 4 8 0.0455 0 0.0455 0 100 0 4 9 0.0455 00.0455 0 100 0 4 10 0.0455 0 0.0455 0 100 0 4 11 0.0455 0 0.0455 0 100 04 12 0.0455 0 0.0455 0 100 0 4 13 0.0455 0 0.0455 0 100 0 4 14 0.04550.625 0.6705 0 6.79 93.21 4 15 0.0455 0 0.6705 93.21 6.79 0 4 16 0 00.1275 0 100 0 5 1 0.0524 0 0.0524 0 100 0 5 2 0.0524 0 0.0524 0 100 0 53 0.0524 0 0.0524 0 100 0 5 4 0.0524 0 0.0524 0 100 0 5 5 0.0524 00.0524 0 100 0 5 6 0.0524 0 0.0524 0 100 0 5 7 0.0524 0 0.0524 0 100 0 58 0.0524 0 0.0524 0 100 0 5 9 0.0524 0 0.0524 0 100 0 5 10 0.0524 00.0524 0 100 0 5 11 0.0524 0 0.0524 0 100 0 5 12 0.0524 0 0.0524 0 100 05 13 0.0524 0 0.0524 0 100 0 5 14 0.0524 0.625 0.6774 0 7.73 92.27 5 150.0524 0 0.6774 92.27 7.73 0 5 16 0 0 0 0 0 0 6 1 0.0592 0 0.0592 0 1000 6 2 0.0592 0 0.0592 0 100 0 6 3 0.0592 0 0.0592 0 100 0 6 4 0.0592 00.0592 0 100 0 6 5 0.0592 0 0.0592 0 100 0 6 6 0.0592 0 0.0592 0 100 0 67 0.0592 0 0.0592 0 100 0 6 8 0.0592 0 0.0592 0 100 0 6 9 0.0592 00.0592 0 100 0 6 10 0.0592 0 0.0592 0 100 0 6 11 0.0592 0 0.0592 0 100 05 12 0.0592 0 0.0592 0 100 0 6 13 0.0592 0 0.0592 0 100 0 6 14 0.05920.625 0.6842 0 8.65 91.35 6 15 0.0592 0 0.6842 91.35 8.65 0 6 16 0 0 0 00 0 7 1 0.066 0 0.066 0 100 0 7 2 0.066 0 0.066 0 100 0 7 3 0.066 00.066 0 100 0 7 4 0.066 0 0.066 0 100 0 7 5 0.066 0 0.066 0 100 0 7 60.066 0 0.066 0 100 0 7 7 0.066 0 0.066 0 100 0 7 8 0.066 0 0.066 0 1000 7 9 0.066 0 0.066 0 100 0 7 10 0.066 0 0.066 0 100 0 7 11 0.066 00.066 0 100 0 7 12 0.066 0 0.066 0 100 0 7 13 0.066 0 0.066 0 100 0 7 140.066 0.625 0.691 0 9.55 90.45 7 15 0.066 0 0.691 90.45 9.55 0 7 16 0 00.1275 0 100 0 8 1 0.0729 0 0.0729 0 100 0 8 2 0.0729 0 0.0729 0 100 0 83 0.0729 0 0.0729 0 100 0 8 4 0.0729 0 0.0729 0 100 0 8 5 0.0729 00.0729 0 100 0 8 6 0.0729 0 0.0729 0 100 0 8 7 0.0729 0 0.0729 0 100 0 88 0.0729 0 0.0729 0 100 0 8 9 0.0729 0 0.0729 0 100 0 8 10 0.0729 00.0729 0 100 0 8 11 0.0729 0 0.0729 0 100 0 8 12 0.0729 0 0.0729 0 100 08 13 0.0729 0 0.0729 0 100 0 8 14 0.0729 0.625 0.6979 0 10.44 89.56 8 150.0729 0 0.6979 89.56 10.44 0 8 16 0 0 0 0 0 0 9 1 0.0797 0 0.0797 0 1000 9 2 0.0797 0 0.0797 0 100 0 9 3 0.0797 0 0.0797 0 100 0 9 4 0.0797 00.0797 0 100 0 9 5 0.0797 0 0.0797 0 100 0 9 6 0.0797 0 0.0797 0 100 0 97 0.0797 0 0.0797 0 100 0 9 8 0.0797 0 0.0797 0 100 0 9 9 0.0797 00.0797 0 100 0 9 10 0.0797 0 0.0797 0 100 0 9 11 0.0797 0 0.0797 0 100 09 12 0.0797 0 0.0797 0 100 0 9 13 0.0797 0 0.0797 0 100 0 9 14 0.07970.625 0.7047 0 11.31 88.69 9 15 0.0797 0 0.7047 88.69 11.31 0 9 16 0 0 00 0 0 10 1 0.0865 0 0.0865 0 100 0 10 2 0.0865 0 0.0865 0 100 0 10 30.0865 0 0.0865 0 100 0 10 4 0.0865 0 0.0865 0 100 0 10 5 0.0865 00.0865 0 100 0 10 6 0.0865 0 0.0865 0 100 0 10 7 0.0865 0 0.0865 0 100 010 8 0.0865 0 0.0865 0 100 0 10 9 0.0865 0 0.0865 0 100 0 10 10 0.0865 00.0865 0 100 0 10 11 0.0865 0 0.0865 0 100 0 10 12 0.0865 0 0.0865 0 1000 10 13 0.0865 0 0.0865 0 100 0 10 14 0.0865 0.625 0.7115 0 12.16 87.8410 15 0.0865 0 0.7115 87.84 12.16 0 10 16 0 0 0.1275 0 100 0 11 1 0.09330 0.0933 0 100 0 11 2 0.0933 0 0.0933 0 100 0 11 3 0.0933 0 0.0933 0 1000 11 4 0.0933 0 0.0933 0 100 0 11 5 0.0933 0 0.0933 0 100 0 11 6 0.09330 0.0933 0 100 0 11 7 0.0933 0 0.0933 0 100 0 11 8 0.0933 0 0.0933 0 1000 11 9 0.0933 0 0.0933 0 100 0 11 10 0.0933 0 0.0933 0 100 0 11 110.0933 0 0.0933 0 100 0 11 12 0.0933 0 0.0933 0 100 0 11 13 0.0933 00.0933 0 100 0 11 14 0.0933 0.625 0.7183 0 12.99 87.01 11 15 0.0933 00.7183 87.01 12.99 0 11 16 0 0 0 0 0 0 12 1 0.1002 0 0.1002 0 100 0 12 20.1002 0 0.1002 0 100 0 12 3 0.1002 0 0.1002 0 100 0 12 4 0.1002 00.1002 0 100 0 12 5 0.1002 0 0.1002 0 100 0 12 6 0.1002 0 0.1002 0 100 012 7 0.1002 0 0.1002 0 100 0 12 8 0.1002 0 0.1002 0 100 0 12 9 0.1002 00.1002 0 100 0 12 10 0.1002 0 0.1002 0 100 0 12 11 0.1002 0 0.1002 0 1000 12 12 0.1002 0 0.1002 0 100 0 12 13 0.1002 0 0.1002 0 100 0 12 140.1002 0.625 0.7252 0 13.81 86.19 12 15 0.1002 0 0.7252 86.19 13.81 0 1216 0 0 0 0 0 0 13 1 0.107 0 0.107 0 100 0 13 2 0.107 0 0.107 0 100 0 133 0.107 0 0.107 0 100 0 13 4 0.107 0 0.107 0 100 0 13 5 0.107 0 0.107 0100 0 13 6 0.107 0 0.107 0 100 0 13 7 0.107 0 0.107 0 100 0 13 8 0.107 00.107 0 100 0 13 9 0.107 0 0.107 0 100 0 13 10 0.107 0 0.107 0 100 0 1311 0.107 0 0.107 0 100 0 13 12 0.107 0 0.107 0 100 0 13 13 0.107 0 0.1070 100 0 13 14 0.107 0.625 0.732 0 14.62 85.38 13 15 0.107 0 0.732 85.3814.62 0 13 16 0 0 0.1275 0 100 0 14 1 0.1138 0 0.1138 0 100 0 14 20.1138 0 0.1138 0 100 0 14 3 0.1138 0 0.1138 0 100 0 14 4 0.1138 00.1138 0 100 0 14 5 0.1138 0 0.1138 0 100 0 14 6 0.1138 0 0.1138 0 100 014 7 0.1138 0 0.1138 0 100 0 14 8 0.1138 0 0.1138 0 100 0 14 9 0.1138 00.1138 0 100 0 14 10 0.1138 0 0.1138 0 100 0 14 11 0.1138 0 0.1138 0 1000 14 12 0.1138 0 0.1138 0 100 0 14 13 0.1138 0 0.1138 0 100 0 14 140.1138 0.625 0.7388 0 15.41 84.59 14 15 0.1138 0 0.7388 84.59 15.41 0 1416 0 0 0 0 0 0 15 1 0.1207 0 0.1207 0 100 0 15 2 0.1207 0 0.1207 0 100 015 3 0.1207 0 0.1207 0 100 0 15 4 0.1207 0 0.1207 0 100 0 15 5 0.1207 00.1207 0 100 0 15 6 0.1207 0 0.1207 0 100 0 15 7 0.1207 0 0.1207 0 100 015 8 0.1207 0 0.1207 0 100 0 15 9 0.1207 0 0.1207 0 100 0 15 10 0.1207 00.1207 0 100 0 15 11 0.1207 0 0.1207 0 100 0 15 12 0.1207 0 0.1207 0 1000 15 13 0.1207 0 0.1207 0 100 0 15 14 0.1207 0.625 0.7457 0 16.18 83.8215 15 0.1207 0 0.7457 83.82 16.18 0 15 16 0 0 0 0 0 0 16 1 0.1275 00.1275 0 100 0 16 2 0.1275 0 0.1275 0 100 0 16 3 0.1275 0 0.1275 0 100 016 4 0.1275 0 0.1275 0 100 0 16 5 0.1275 0 0.1275 0 100 0 16 6 0.1275 00.1275 0 100 0 16 7 0.1275 0 0.1275 0 100 0 16 8 0.1275 0 0.1275 0 100 016 9 0.1275 0 0.1275 0 100 0 16 10 0.1275 0 0.1275 0 100 0 16 11 0.12750 0.1275 0 100 0 16 12 0.1275 0 0.1275 0 100 0 16 13 0.1275 0 0.1275 0100 0 16 14 0.1275 0.625 0.7525 0 16.94 83.06 16 15 0.1275 0 0.752583.06 16.94 0 16 16 0 0 0.1275 0 100 0 Tem- pera- ture: 300 C. Pt1.0%/ RC COCONV H2OCONV CO2PROD CO2PERPROD CH4PROD Zr02_std LaNO33 1 1 26.041213.6761 0.7608 27.4327 0.1592 0.1275 0 1 2 1.9716 2.4686 0.0066 0.23860.0092 0 0 1 3 0.3229 0.3952 −0.0391 −1.4081 0.0062 0 0 1 4 0.64170.8578 −0.0504 −1.8187 −0.0005 0 0 1 5 0.173 0.5233 −0.0449 −1.61830.0024 0 0 1 6 0.3624 0.0747 −0.0376 −1.3546 −0.0039 0 0 1 7 26.15712.3934 0.797 28.7383 0.1699 0.1275 0 1 8 3.5333 0.2801 −0.0585 −2.108−0.0107 0 0 1 9 −1.8657 −3.8002 −0.0104 −0.375 0.0197 0 0 1 10 2.5920.129 −0.014 −0.5051 −0.0253 0 0 1 11 −3.1613 −1.397 −0.0273 −0.98580.0043 0 0 1 12 −0.5382 −0.741 −0.0195 −0.7042 −0.0352 0 0 1 13 25.29312.9331 0.8097 29.194 0.1597 0.1275 0 1 14 0.8774 0.3654 −0.018 −0.6480.0052 0 0 1 15 −1.2793 0.1383 −0.0181 −0.6543 0.0027 0 0 1 16 25.673512.143 0.7277 26.2368 0.1566 0.1275 0 2 1 14.8766 10.2106 0.3917 14.12170.0524 0 0 2 2 20.4545 14.6181 0.746 26.8969 0.1088 0 0 2 3 19.935212.3858 0.6977 25.1579 0.1196 0 0 2 4 16.0396 10.1097 0.6511 23.47680.109 0 0 2 5 15.904 10.2101 0.4597 16.5765 0.0626 0 0 2 6 14.99159.8692 0.3995 14.4034 0.0662 0 0 2 7 6.2101 5.2473 0.1852 6.6763 0.02520 0 2 8 9.4972 5.8339 0.283 10.205 0.0496 0 0 2 9 21.1669 13.9111 0.643523.2016 0.0932 0 0 2 10 8.0932 5.8934 0.2958 10.6661 0.0493 0 0 2 110.4906 0.3109 −0.0754 −2.7173 0.0004 0 0 2 12 12.7979 8.96 0.445 16.04390.0703 0 0 2 13 1.7683 2.1621 0.0286 1.0326 0.0176 0 0 2 14 11.50498.9483 0.3603 12.9899 0.0656 0 0 2 15 19.2509 11.5249 0.6541 23.58490.0881 0 0.625 2 16 −2.2275 0.1022 0.0038 0.136 0.001 0 0 3 1 19.562513.7405 0.7553 27.2322 0.1169 0 0 3 2 23.3448 16.4986 0.7782 28.05990.1055 0 0 3 3 20.2746 14.4888 0.7447 26.8513 0.1236 0 0 3 4 21.04214.6567 0.5975 21.5435 0.0868 0 0 3 5 15.227 11.3009 0.5184 18.69310.0896 0 0 3 6 16.2981 13.1574 0.4916 17.7266 0.0804 0 0 3 7 7.53187.7146 0.2177 7.8495 0.0364 0 0 3 8 14.1025 10.9954 0.419 15.1061 0.06280 0 3 9 20.9253 15.3432 0.7024 25.3266 0.1019 0 0 3 10 13.728 11.16050.4466 16.1033 0.0679 0 0 3 11 −1.0656 0.7638 −0.03 −1.0824 −0.001 0 0 312 12.0316 9.0087 0.4143 14.9372 0.064 0 0 3 13 2.3735 2.427 0.04721.7003 0.0158 0 0 3 14 10.011 6.6184 0.4321 15.5784 0.078 0 0 3 1517.1288 11.9418 0.6936 25.0081 0.1016 0 0.625 3 16 −0.0207 −0.00560.0564 2.0341 −0.003 0 0 4 1 23.9972 15.9845 0.7717 27.8233 0.119 0 0 42 24.3635 16.2531 0.7072 25.5007 0.1199 0 0 4 3 21.4425 14.1432 0.749827.0362 0.1265 0 0 4 4 19.4479 12.996 0.6822 24.5996 0.107 0 0 4 516.0527 11.3163 0.5819 20.98 0.0935 0 0 4 6 17.5309 11.186 0.5671 20.4470.0842 0 0 4 7 8.0993 5.7381 0.3374 12.166 0.0503 0 0 4 8 14.119 9.81070.5489 19.7929 0.0801 0 0 4 9 23.2762 14.9011 0.7786 28.0723 0.1033 0 04 10 14.7194 10.4363 0.5718 20.6185 0.08 0 0 4 11 1.1453 0.3882 −0.067−2.4162 −0.0168 0 0 4 12 12.7656 8.8311 0.4759 17.1582 0.0689 0 0 4 134.4502 1.323 0.0072 0.2593 0.0135 0 0 4 14 13.3844 9.4729 0.4141 14.93110.0687 0 0 4 15 20.7018 14.4153 0.6795 24.5002 0.0932 0 0.625 4 1626.3093 12.5646 0.7405 26.6988 0.1561 0.1275 0 5 1 21.4105 14.40670.7125 25.6898 0.11 0 0 5 2 22.1022 14.8036 0.819 29.5304 0.1282 0 0 5 322.5933 14.8442 0.7244 26.1201 0.1233 0 0 5 4 21.0057 13.8057 0.691124.9201 0.1153 0 0 5 5 17.672 12.2393 0.5728 20.6522 0.0902 0 0 5 616.0245 11.7967 0.5902 21.2789 0.0941 0 0 5 7 8.682 6.8022 0.35 12.61850.0569 0 0 5 8 16.2047 10.7313 0.5656 20.3921 0.0857 0 0 5 9 21.072914.0649 0.7974 28.7515 0.124 0 0 5 10 18.1655 12.1093 0.6249 22.53230.094 0 0 5 11 −3.2789 −1.8833 0.0173 0.625 −0.017 0 0 5 12 12.13767.6528 0.5085 18.3339 0.0689 0 0 5 13 2.8719 1.6064 0.0398 1.4347 0.02320 0 5 14 11.6313 7.1984 0.3756 13.5442 0.064 0 0 5 15 18.7077 12.34220.6784 24.4596 0.1017 0 0.625 5 16 −0.923 0.6423 0.0024 0.0871 −0.0005 00 6 1 22.0063 14.1082 0.7772 28.0216 0.121 0 0 6 2 23.7522 14.42510.8181 29.4983 0.1363 0 0 6 3 23.7349 12.7968 0.778 28.0518 0.1487 0 0 64 21.7688 12.1769 0.7488 27.0006 0.1335 0 0 6 5 18.6185 12.368 0.629222.6862 0.1057 0 0 6 6 17.435 11.7025 0.6457 23.2833 0.0997 0 0 6 79.5496 7.4033 0.4005 14.4418 0.0656 0 0 6 8 18.8345 12.608 0.602 21.70770.0895 0 0 6 9 22.7783 14.5707 0.7858 28.3319 0.1268 0 0 6 10 14.28899.3319 0.4808 17.3344 0.0626 0 0 6 11 −1.4423 −3.1898 0.0072 0.2597−0.0242 0 0 6 12 14.6391 9.1343 0.5169 18.6393 0.0784 0 0 6 13 1.39240.1849 0.1067 3.8458 0.0254 0 0 6 14 12.4467 7.9011 0.47 16.947 0.0796 00 6 15 20.5551 12.4877 0.7241 26.1085 0.1086 0 0.625 6 16 1.8224 1.91940.0293 1.0577 −0.001 0 0 7 1 20.1793 13.5157 0.7141 25.7483 0.1062 0 0 72 23.9199 15.0715 0.7923 28.5691 0.1334 0 0 7 3 24.0921 13.8724 0.770427.7794 0.1489 0 0 7 4 22.4883 13.3333 0.7472 26.9401 0.1331 0 0 7 518.3753 10.967 0.6933 24.9964 0.1147 0 0 7 6 19.1636 11.8882 0.59421.4179 0.0973 0 0 7 7 11.6242 8.7829 0.358 12.9075 0.0589 0 0 7 818.9461 11.9304 0.6075 21.9057 0.0865 0 0 7 9 20.8727 13.268 0.858130.9391 0.1366 0 0 7 10 19.7469 12.533 0.627 22.6084 0.0889 0 0 7 110.2661 −1.0746 −0.0206 −0.7417 −0.0241 0 0 7 12 14.9635 8.7674 0.511718.4485 0.0776 0 0 7 13 2.473 1.1259 0.0915 3.3004 0.0134 0 0 7 1410.4908 6.4436 0.4097 14.774 0.0771 0 0 7 15 17.9387 11.3159 0.733526.449 0.109 0 0.625 7 16 24.6649 12.1883 0.7892 28.4564 0.1735 0.1275 08 1 20.4072 13.9072 0.7031 25.3521 0.1107 0 0 8 2 23.2299 15.5533 0.807829.1272 0.1368 0 0 8 3 24.3029 13.9797 0.7799 28.1203 0.1564 0 0 8 422.2113 14.5975 0.7495 27.0256 0.1425 0 0 8 5 18.1577 13.0692 0.694325.034 0.1167 0 0 8 6 16.4584 11.241 0.6799 24.5135 0.1128 0 0 8 711.3178 9.6452 0.4321 15.5795 0.0596 0 0 8 8 20.8336 14.4605 0.645723.2815 0.0922 0 0 8 9 23.346 15.3942 0.8346 30.0941 0.1169 0 0 8 1020.3283 13.3467 0.6964 25.1102 0.1063 0 0 8 11 6.0017 3.7447 0.23448.4523 0.0402 0 0 8 12 14.0669 9.2173 0.572 20.6246 0.0862 0 0 8 130.4343 −0.3379 0.1029 3.7103 0.0224 0 0 8 14 12.9196 8.2041 0.468916.9054 0.0749 0 0 8 15 20.3025 12.6472 0.6618 23.8639 0.1 0 0.625 8 160.7273 0.7062 −0.0175 −0.63 −0.0087 0 0 9 1 19.0866 13.801 0.695625.0805 0.1067 0 0 9 2 23.4011 15.4022 0.8062 29.0677 0.1362 0 0 9 324.2636 14.0356 0.8069 29.094 0.1585 0 0 9 4 23.0618 13.7204 0.760327.4122 0.137 0 0 9 5 19.2953 12.3324 0.6838 24.6546 0.1191 0 0 9 616.4524 11.6941 0.5833 21.033 0.0966 0 0 9 7 8.8155 6.193 0.4081 14.71540.0678 0 0 9 8 18.3421 12.4823 0.6492 23.4094 0.095 0 0 9 9 22.557115.4221 0.8241 29.7153 0.1201 0 0 9 10 18.2863 13.1397 0.6724 24.24440.0988 0 0 9 11 −1.5339 −0.5868 −0.0006 −0.0218 −0.0198 0 0 9 12 13.96029.1693 0.5547 20.0022 0.0819 0 0 9 13 1.1827 1.2849 0.1107 3.9916 0.00240 0 9 14 10.2757 6.1288 0.3969 14.3106 0.0711 0 0 9 15 19.4095 11.48490.732 26.3918 0.1116 0 0.625 9 16 −0.4746 0.3 0.0649 2.3389 0.0106 0 010 1 19.6155 13.2592 0.7151 25.784 0.1137 0 0 10 2 24.4255 14.21140.8452 30.474 0.1541 0 0 10 3 25.1167 12.0723 0.8229 29.6706 0.1783 0 010 4 23.9367 12.0867 0.8302 29.934 0.1595 0 0 10 5 20.499 11.2772 0.694925.0561 0.1257 0 0 10 6 18.4277 10.342 0.652 23.5077 0.1136 0 0 10 710.6829 8.2331 0.4943 17.8212 0.0797 0 0 10 8 21.0351 13.5697 0.693425.0025 0.1016 0 0 10 9 23.3546 15.5724 0.8319 29.9961 0.1265 0 0 10 1020.2733 13.206 0.7226 26.0547 0.1094 0 0 10 11 −2.2709 −1.6818 −0.003−0.1081 −0.0191 0 0 10 12 15.5394 9.154 0.5767 20.7948 0.0875 0 0 10 132.338 0.6958 0.1166 4.204 0.0286 0 0 10 14 11.8371 7.0502 0.4485 16.17020.0781 0 0 10 15 18.9643 11.9052 0.7159 25.8125 0.1082 0 0.625 10 1623.3683 12.0328 0.7792 28.0962 0.1577 0.1275 0 11 1 18.6802 11.57420.6796 24.5045 0.1057 0 0 11 2 25.0222 13.9863 0.8039 28.9852 0.1512 0 011 3 25.6394 13.1215 0.8122 29.2838 0.1687 0 0 11 4 24.6744 14.51830.7802 28.132 0.1536 0 0 11 5 19.3295 12.6135 0.685 24.6995 0.1225 0 011 6 18.7665 11.7823 0.6491 23.4044 0.1112 0 0 11 7 12.0459 8.262 0.466916.8355 0.0746 0 0 11 8 19.7356 12.2924 0.7225 26.0526 0.1072 0 0 11 923.3494 14.4131 0.8518 30.7139 0.1298 0 0 11 10 19.1323 12.6849 0.709425.5779 0.105 0 0 11 11 −0.9895 −0.2695 −0.004 −0.1435 −0.0127 0 0 11 1214.8304 10.1963 0.582 20.9867 0.0899 0 0 11 13 2.208 2.5587 0.10293.7107 0.0204 0 0 11 14 10.9763 6.4266 0.3918 14.1258 0.0707 0 0 11 1518.1906 10.6621 0.698 25.1685 0.106 0 0.625 11 16 −0.9643 −0.7161 0.03921.4143 −0.0048 0 0 12 1 15.4588 10.1833 0.5953 21.4632 0.1001 0 0 12 224.7319 13.6012 0.8478 30.5688 0.161 0 0 12 3 26.8912 12.8758 0.800828.8754 0.1851 0 0 12 4 24.6558 12.9216 0.8196 29.5504 0.1758 0 0 12 520.5267 12.1018 0.7215 26.0139 0.1329 0 0 12 6 18.4287 11.4481 0.681124.5589 0.1172 0 0 12 7 13.4393 9.372 0.4909 17.6995 0.0793 0 0 12 821.0809 13.9911 0.7512 27.0875 0.111 0 0 12 9 23.772 15.0448 0.851730.7084 0.1339 0 0 12 10 19.8095 12.8912 0.7381 26.6137 0.1093 0 0 12 11−1.4941 −1.399 −0.0134 −0.4846 −0.018 0 0 12 12 16.0743 10.6539 0.597721.5507 0.092 0 0 12 13 2.0581 1.6359 0.1105 3.986 0.0298 0 0 12 1410.744 6.4761 0.4184 15.0852 0.076 0 0 12 15 18.2843 10.3265 0.697525.1492 0.112 0 0.625 12 16 −0.4083 −1.1083 0.0632 2.2805 0.02 0 0 13 117.3784 11.3659 0.6531 23.5471 0.1026 0 0 13 2 24.8735 13.9698 0.864531.1714 0.1634 0 0 13 3 26.731 13.2379 0.8304 29.9397 0.1799 0 0 13 425.0125 13.3208 0.8199 29.5626 0.1706 0 0 13 5 20.9959 12.5637 0.725.2389 0.1263 0 0 13 6 19.7859 13.0643 0.6384 23.0182 0.1112 0 0 13 712.7701 8.6484 0.4737 17.0786 0.0821 0 0 13 8 19.9798 12.3643 0.742126.7561 0.1113 0 0 13 9 23.9004 15.4262 0.8368 30.1725 0.1326 0 0 13 1020.1688 14.395 0.7685 27.7093 0.1134 0 0 13 11 −1.5531 −0.2131 0.00030.0093 −0.0139 0 0 13 12 16.261 10.9519 0.6007 21.66 0.0928 0 0 13 132.1579 1.7026 0.1307 4.7131 0.0287 0 0 13 14 10.3449 7.0881 0.401314.4697 0.0725 0 0 13 15 17.9906 12.3676 0.6892 24.8485 0.1057 0 0.62513 16 24.9296 12.3107 0.7853 28.3135 0.1895 0.1275 0 14 1 19.7006 13.8950.7196 25.9447 0.1225 0 0 14 2 24.628 13.7864 0.8645 31.1715 0.1715 0 014 3 27.0603 12.7211 0.8226 29.6605 0.2007 0 0 14 4 24.9719 12.0514 0.8329.9259 0.1896 0 0 14 5 20.0669 11.3486 0.7334 26.4431 0.1416 0 0 14 619.3148 11.3116 0.7073 25.5033 0.128 0 0 14 7 13.0698 9.2496 0.517818.6703 0.0862 0 0 14 8 21.4825 14.0766 0.7634 27.5263 0.1153 0 0 14 923.8379 15.3459 0.8607 31.0347 0.1367 0 0 14 10 21.5278 13.8928 0.785128.3081 0.1137 0 0 14 11 −2.1621 −1.2165 −0.0091 −0.3271 −0.0078 0 0 1412 17.3041 11.5725 0.646 23.2923 0.0958 0 0 14 13 1.949 2.0565 0.08963.2302 0.028 0 0 14 14 9.3689 6.5087 0.3449 12.4353 0.0636 0 0 14 1518.4324 12.0276 0.6914 24.9297 0.1067 0 0.625 14 16 −0.7558 −0.68980.0165 0.5934 0.0011 0 0 15 1 18.1472 11.9418 0.6987 25.1939 0.1082 0 015 2 24.7631 13.6604 0.8641 31.1563 0.1697 0 0 15 3 26.1211 11.82270.834 30.0705 0.2037 0 0 15 4 24.5677 11.9552 0.7923 28.5692 0.1875 0 015 5 20.0898 11.474 0.7193 25.9371 0.144 0 0 15 6 19.3675 11.6613 0.682224.5972 0.1254 0 0 15 7 12.9911 8.3415 0.5124 18.477 0.0905 0 0 15 819.4851 12.9013 0.711 25.6353 0.1146 0 0 15 9 23.6077 14.5462 0.861831.074 0.1436 0 0 15 10 21.2589 13.7735 0.7922 28.5624 0.1207 0 0 15 11−1.3789 −1.3203 0.0019 0.0686 −0.0106 0 0 15 12 16.8366 10.3498 0.648923.3953 0.1014 0 0 15 13 2.5374 0.8067 0.138 4.9742 0.0357 0 0 15 1411.1396 7.0915 0.4088 14.741 0.0773 0 0 15 15 17.5426 10.4944 0.704525.4019 0.1136 0 0.625 15 16 −0.4051 −0.4444 0.0729 2.6294 0.0112 0 0 161 15.0725 8.0994 0.5869 21.1613 0.0985 0 0 16 2 24.67 8.6858 0.700925.2716 0.2051 0 0 16 3 27.4278 6.3099 0.707 25.4923 0.2645 0 0 16 424.8032 6.1186 0.6967 25.1217 0.2372 0 0 16 5 20.9479 7.854 0.670724.1843 0.1784 0 0 16 6 19.4346 9.972 0.6893 24.8548 0.1408 0 0 16 714.3144 8.9315 0.5183 18.6864 0.0889 0 0 16 8 20.6449 13.6205 0.702325.3217 0.1142 0 0 16 9 24.2561 14.785 0.854 30.7919 0.1506 0 0 16 1021.0486 14.0733 0.6995 25.2209 0.1084 0 0 16 11 −2.2759 −0.0846 0.04131.4879 0.024 0 0 16 12 17.1423 10.7518 0.5869 21.1613 0.0898 0 0 16 133.0092 2.0883 0.2069 7.4586 0.0432 0 0 16 14 12.8714 7.6083 0.514218.5415 0.1069 0 0 16 15 17.5841 9.9481 0.6294 22.6946 0.129 0 0.625 1616 25.0686 11.1805 0.8288 29.884 0.1822 0.1275 0 Tem- pera- ture: 300 C.Sum_(—) mol % mol % mol % R C PtNH32NO22 ZrONO32 micromols La Pt Zr 1 10 0 0.1275 0 100 0 1 2 0 0 0 0 0 0 1 3 0 0 0 0 0 0 1 4 0 0 0 0 0 0 1 5 00 0 0 0 0 1 6 0 0 0 0 0 0 1 7 0 0 0.1275 0 100 0 1 8 0 0 0 0 0 0 1 9 0 00 0 0 0 1 10 0 0 0 0 0 0 1 11 0 0 0 0 0 0 1 12 0 0 0 0 0 0 1 13 0 00.1275 0 100 0 1 14 0 0 0 0 0 0 1 15 0 0 0 0 0 0 1 16 0 0 0.1275 0 100 02 1 0.0319 0 0.0319 0 100 0 2 2 0.0319 0 0.0319 0 100 0 2 3 0.0319 00.0319 0 100 0 2 4 0.0319 0 0.0319 0 100 0 2 5 0.0319 0 0.0319 0 100 0 26 0.0319 0 0.0319 0 100 0 2 7 0.0319 0 0.0319 0 100 0 2 8 0.0319 00.0319 0 100 0 2 9 0.0319 0 0.0319 0 100 0 2 10 0.0319 0 0.0319 0 100 02 11 0.0319 0 0.0319 0 100 0 2 12 0.0319 0 0.0319 0 100 0 2 13 0.0319 00.0319 0 100 0 2 14 0.0319 0.625 0.6569 0 4.85 95.15 2 15 0.0319 00.6569 95.15 4.85 0 2 16 0 0 0 0 0 0 3 1 0.0387 0 0.0387 0 100 0 3 20.0387 0 0.0387 0 100 0 3 3 0.0387 0 0.0387 0 100 0 3 4 0.0387 0 0.03870 100 0 3 5 0.0387 0 0.0387 0 100 0 3 6 0.0387 0 0.0387 0 100 0 3 70.0387 0 0.0387 0 100 0 3 8 0.0387 0 0.0387 0 100 0 3 9 0.0387 0 0.03870 100 0 3 10 0.0387 0 0.0387 0 100 0 3 11 0.0387 0 0.0387 0 100 0 3 120.0387 0 0.0387 0 100 0 3 13 0.0387 0 0.0387 0 100 0 3 14 0.0387 0.6250.6637 0 5.83 94.17 3 15 0.0387 0 0.6637 94.17 5.83 0 3 16 0 0 0 0 0 0 41 0.0455 0 0.0455 0 100 0 4 2 0.0455 0 0.0455 0 100 0 4 3 0.0455 00.0455 0 100 0 4 4 0.0455 0 0.0455 0 100 0 4 5 0.0455 0 0.0455 0 100 0 46 0.0455 0 0.0455 0 100 0 4 7 0.0455 0 0.0455 0 100 0 4 8 0.0455 00.0455 0 100 0 4 9 0.0455 0 0.0455 0 100 0 4 10 0.0455 0 0.0455 0 100 04 11 0.0455 0 0.0455 0 100 0 4 12 0.0455 0 0.0455 0 100 0 4 13 0.0455 00.0455 0 100 0 4 14 0.0455 0.625 0.6705 0 6.79 93.21 4 15 0.0455 00.6705 93.21 6.79 0 4 16 0 0 0.1275 0 100 0 5 1 0.0524 0 0.0524 0 100 05 2 0.0524 0 0.0524 0 100 0 5 3 0.0524 0 0.0524 0 100 0 5 4 0.0524 00.0524 0 100 0 5 5 0.0524 0 0.0524 0 100 0 5 6 0.0524 0 0.0524 0 100 0 57 0.0524 0 0.0524 0 100 0 5 8 0.0524 0 0.0524 0 100 0 5 9 0.0524 00.0524 0 100 0 5 10 0.0524 0 0.0524 0 100 0 5 11 0.0524 0 0.0524 0 100 05 12 0.0524 0 0.0524 0 100 0 5 13 0.0524 0 0.0524 0 100 0 5 14 0.05240.625 0.6774 0 7.73 92.27 5 15 0.0524 0 0.6774 92.27 7.73 0 5 16 0 0 0 00 0 6 1 0.0592 0 0.0592 0 100 0 6 2 0.0592 0 0.0592 0 100 0 6 3 0.0592 00.0592 0 100 0 6 4 0.0592 0 0.0592 0 100 0 6 5 0.0592 0 0.0592 0 100 0 66 0.0592 0 0.0592 0 100 0 6 7 0.0592 0 0.0592 0 100 0 6 8 0.0592 00.0592 0 100 0 6 9 0.0592 0 0.0592 0 100 0 6 10 0.0592 0 0.0592 0 100 06 11 0.0592 0 0.0592 0 100 0 6 12 0.0592 0 0.0592 0 100 0 6 13 0.0592 00.0592 0 100 0 6 14 0.0592 0.625 0.6842 0 8.65 91.35 6 15 0.0592 00.6842 91.35 8.65 0 6 16 0 0 0 0 0 0 7 1 0.066 0 0.066 0 100 0 7 2 0.0660 0.066 0 100 0 7 3 0.066 0 0.066 0 100 0 7 4 0.066 0 0.066 0 100 0 7 50.066 0 0.066 0 100 0 7 6 0.066 0 0.066 0 100 0 7 7 0.066 0 0.066 0 1000 7 8 0.066 0 0.066 0 100 0 7 9 0.066 0 0.066 0 100 0 7 10 0.066 0 0.0660 100 0 7 11 0.066 0 0.066 0 100 0 7 12 0.066 0 0.066 0 100 0 7 13 0.0660 0.066 0 100 0 7 14 0.066 0.625 0.691 0 9.55 90.45 7 15 0.066 0 0.69190.45 9.55 0 7 16 0 0 0.1275 0 100 0 8 1 0.0729 0 0.0729 0 100 0 8 20.0729 0 0.0729 0 100 0 8 3 0.0729 0 0.0729 0 100 0 8 4 0.0729 0 0.07290 100 0 8 5 0.0729 0 0.0729 0 100 0 8 6 0.0729 0 0.0729 0 100 0 8 70.0729 0 0.0729 0 100 0 8 8 0.0729 0 0.0729 0 100 0 8 9 0.0729 0 0.07290 100 0 8 10 0.0729 0 0.0729 0 100 0 8 11 0.0729 0 0.0729 0 100 0 8 120.0729 0 0.0729 0 100 0 8 13 0.0729 0 0.0729 0 100 0 8 14 0.0729 0.6250.6979 0 10.44 89.56 8 15 0.0729 0 0.6979 89.56 10.44 0 8 16 0 0 0 0 0 09 1 0.0797 0 0.0797 0 100 0 9 2 0.0797 0 0.0797 0 100 0 9 3 0.0797 00.0797 0 100 0 9 4 0.0797 0 0.0797 0 100 0 9 5 0.0797 0 0.0797 0 100 0 96 0.0797 0 0.0797 0 100 0 9 7 0.0797 0 0.0797 0 100 0 9 8 0.0797 00.0797 0 100 0 9 9 0.0797 0 0.0797 0 100 0 9 10 0.0797 0 0.0797 0 100 09 11 0.0797 0 0.0797 0 100 0 9 12 0.0797 0 0.0797 0 100 0 9 13 0.0797 00.0797 0 100 0 9 14 0.0797 0.625 0.7047 0 11.31 88.69 9 15 0.0797 00.7047 88.69 11.31 0 9 16 0 0 0 0 0 0 10 1 0.0865 0 0.0865 0 100 0 10 20.0865 0 0.0865 0 100 0 10 3 0.0865 0 0.0865 0 100 0 10 4 0.0865 00.0865 0 100 0 10 5 0.0865 0 0.0865 0 100 0 10 6 0.0865 0 0.0865 0 100 010 7 0.0865 0 0.0865 0 100 0 10 8 0.0865 0 0.0865 0 100 0 10 9 0.0865 00.0865 0 100 0 10 10 0.0865 0 0.0865 0 100 0 10 11 0.0865 0 0.0865 0 1000 10 12 0.0865 0 0.0865 0 100 0 10 13 0.0865 0 0.0865 0 100 0 10 140.0865 0.625 0.7115 0 12.16 87.84 10 15 0.0865 0 0.7115 87.84 12.16 0 1016 0 0 0.1275 0 100 0 11 1 0.0933 0 0.0933 0 100 0 11 2 0.0933 0 0.09330 100 0 11 3 0.0933 0 0.0933 0 100 0 11 4 0.0933 0 0.0933 0 100 0 11 50.0933 0 0.0933 0 100 0 11 6 0.0933 0 0.0933 0 100 0 11 7 0.0933 00.0933 0 100 0 11 8 0.0933 0 0.0933 0 100 0 11 9 0.0933 0 0.0933 0 100 011 10 0.0933 0 0.0933 0 100 0 11 11 0.0933 0 0.0933 0 100 0 11 12 0.09330 0.0933 0 100 0 11 13 0.0933 0 0.0933 0 100 0 11 14 0.0933 0.625 0.71830 12.99 87.01 11 15 0.0933 0 0.7183 87.01 12.99 0 11 16 0 0 0 0 0 0 12 10.1002 0 0.1002 0 100 0 12 2 0.1002 0 0.1002 0 100 0 12 3 0.1002 00.1002 0 100 0 12 4 0.1002 0 0.1002 0 100 0 12 5 0.1002 0 0.1002 0 100 012 6 0.1002 0 0.1002 0 100 0 12 7 0.1002 0 0.1002 0 100 0 12 8 0.1002 00.1002 0 100 0 12 9 0.1002 0 0.1002 0 100 0 12 10 0.1002 0 0.1002 0 1000 12 11 0.1002 0 0.1002 0 100 0 12 12 0.1002 0 0.1002 0 100 0 12 130.1002 0 0.1002 0 100 0 12 14 0.1002 0.625 0.7252 0 13.81 86.19 12 150.1002 0 0.7252 86.19 13.81 0 12 16 0 0 0 0 0 0 13 1 0.107 0 0.107 0 1000 13 2 0.107 0 0.107 0 100 0 13 3 0.107 0 0.107 0 100 0 13 4 0.107 00.107 0 100 0 13 5 0.107 0 0.107 0 100 0 13 6 0.107 0 0.107 0 100 0 13 70.107 0 0.107 0 100 0 13 8 0.107 0 0.107 0 100 0 13 9 0.107 0 0.107 0100 0 13 10 0.107 0 0.107 0 100 0 13 11 0.107 0 0.107 0 100 0 13 120.107 0 0.107 0 100 0 13 13 0.107 0 0.107 0 100 0 13 14 0.107 0.6250.732 0 14.62 85.38 13 15 0.107 0 0.732 85.38 14.62 0 13 16 0 0 0.1275 0100 0 14 1 0.1138 0 0.1138 0 100 0 14 2 0.1138 0 0.1138 0 100 0 14 30.1138 0 0.1138 0 100 0 14 4 0.1138 0 0.1138 0 100 0 14 5 0.1138 00.1138 0 100 0 14 6 0.1138 0 0.1138 0 100 0 14 7 0.1138 0 0.1138 0 100 014 8 0.1138 0 0.1138 0 100 0 14 9 0.1138 0 0.1138 0 100 0 14 10 0.1138 00.1138 0 100 0 14 11 0.1138 0 0.1138 0 100 0 14 12 0.1138 0 0.1138 0 1000 14 13 0.1138 0 0.1138 0 100 0 14 14 0.1138 0.625 0.7388 0 15.41 84.5914 15 0.1138 0 0.7388 84.59 15.41 0 14 16 0 0 0 0 0 0 15 1 0.1207 00.1207 0 100 0 15 2 0.1207 0 0.1207 0 100 0 15 3 0.1207 0 0.1207 0 100 015 4 0.1207 0 0.1207 0 100 0 15 5 0.1207 0 0.1207 0 100 0 15 6 0.1207 00.1207 0 100 0 15 7 0.1207 0 0.1207 0 100 0 15 8 0.1207 0 0.1207 0 100 015 9 0.1207 0 0.1207 0 100 0 15 10 0.1207 0 0.1207 0 100 0 15 11 0.12070 0.1207 0 100 0 15 12 0.1207 0 0.1207 0 100 0 15 13 0.1207 0 0.1207 0100 0 15 14 0.1207 0.625 0.7457 0 16.18 83.82 15 15 0.1207 0 0.745783.82 16.18 0 15 16 0 0 0 0 0 0 16 1 0.1275 0 0.1275 0 100 0 16 2 0.12750 0.1275 0 100 0 16 3 0.1275 0 0.1275 0 100 0 16 4 0.1275 0 0.1275 0 1000 16 5 0.1275 0 0.1275 0 100 0 16 6 0.1275 0 0.1275 0 100 0 16 7 0.12750 0.1275 0 100 0 16 8 0.1275 0 0.1275 0 100 0 16 9 0.1275 0 0.1275 0 1000 16 10 0.1275 0 0.1275 0 100 0 16 11 0.1275 0 0.1275 0 100 0 16 120.1275 0 0.1275 0 100 0 16 13 0.1275 0 0.1275 0 100 0 16 14 0.1275 0.6250.7525 0 16.94 83.06 16 15 0.1275 0 0.7525 83.06 16.94 0 16 16 0 00.1275 0 100 0

[0296] TABLE II Tem- pera- ture: 300 C. Pt1.O%/ R C COCONV H2OCONVCO2PROD CO2PERPROD CH4PROD ZrO2_std CeNO33 CoNO32 LaNO33 real real realreal real real real real real real real 1 1 15.7986 12.2353 0.744326.6989 0.2025 0.1275 0 0 0 1 2 −1.6605 −0.4015 0.1746 6.262 0.0427 0 00 0 1 3 −3.3432 −2.8739 0.0909 3.2591 0.0249 0 0 0 0 1 4 −1.5889 −0.75810.0327 1.1725 0.0101 0 0 0 0 1 5 −2.0416 −3.6101 −0.0004 −0.0146 0.00610 0 0 0 1 6 −1.3072 −0.2928 0.0061 0.2203 0.0037 0 0 0 0 1 7 24.164114.6796 0.7194 25.8057 0.2092 0.1275 0 0 0 1 8 1.2706 5.1132 0.03831.3744 0.0043 0 0 0 0 1 9 −1.1139 0.6947 −0.0229 0.8203 −0.0034 0 0 0 01 10 −0.9348 −1.4821 −0.0293 −1.0513 −0.0048 0 0 0 0 1 11 −1.0936−1.3466 −0.0321 1.1501 −0.0057 0 0 0 0 1 12 −0.8945 −2.7312 −0.0352−1.2629 −0.0051 0 0 0 0 1 13 25.7122 17.2709 0.741 26.5814 0.1961 0.12750 0 0 1 14 1.3216 0.8855 0.0278 0.9969 0.0005 0 0 0 0 1 15 −0.33281.9579 −0.047 1.6868 −0.0116 0 0 0 0 1 16 −0.6388 3.8351 −0.0427 −1.5333−0.0128 0 0 0 0 2 1 32.8134 −1.3954 0.4991 17.9018 0.4047 0 0 0.125 0 22 33.7634 −0.7213 0.5627 20.1852 0.398 0 0 0.1964 0 2 3 35.6619 −2.28730.5592 20.0582 0.4282 0 0 0.2679 0 2 4 37.1438 1.718 0.5576 20.00060.441 0 0 0.3393 0 2 5 33.8684 3.0561 0.6422 23.0365 0.3684 0 0 0.4107 02 6 38.7621 −0.7205 0.5983 21.4623 0.4682 0 0 0.4821 0 2 7 40.2724−3.055 0.626 22.4563 0.4782 0 0 0.5536 0 2 8 39.7217 0.3938 0.624822.4111 0.4722 0 0 0.625 0 2 9 42.5893 −5.4627 0.5821 20.8809 0.5336 00.125 0 0 2 10 42.9319 −4.3894 0.5503 19.7403 0.5457 0 0.2083 0 0 2 1144.9469 2.5644 0.4728 16.9586 0.5904 0 0.2917 0 0 2 12 43.7075 3.18940.5096 18.2796 0.5759 0 0.375 0 0 2 13 43.5857 5.9922 0.5426 19.46170.5695 0 0.4583 0 0 2 14 40.9417 1.3479 0.6538 23.4524 0.4792 0 0.5417 00 2 15 40.1679 2.0486 0.5739 20.5869 0.5011 0 0.625 0 0 2 16 1.14321.1008 0.0195 0.7001 0.0042 0 0 0 0 3 1 30.033 1.4197 0.5289 18.97240.3491 0 0 0.125 0 3 2 30.5845 7.6416 0.5106 18.3171 0.3379 0 0 0.1964 03 3 31.5558 6.8985 0.5846 20.9711 0.3398 0 0 0.2679 0 3 4 34.6039−1.0478 0.6413 23.0055 0.3861 0 0 0.3393 0 3 5 34.405 1.0827 0.659223.6444 0.3741 0 0 0.4107 0 3 6 35.4145 8.0388 0.6032 21.6388 0.3881 0 00.4821 0 3 7 37.4154 2.8929 0.6467 23.1968 0.419 0 0 0.5536 0 3 839.1571 3.1565 0.6197 22.2277 0.4582 0 0 0.625 0 3 9 39.1656 −1.04810.6204 22.2537 0.4536 0 0.125 0 0 3 10 40.5621 −2.6868 0.6187 22.19370.4797 0 0.2083 0 0 3 11 39.3799 2.8396 0.6225 22.3281 0.4421 0 0.2917 00 3 12 38.9106 0.6095 0.6545 23.4766 0.4343 0 0.375 0 0 3 13 38.30871.387 0.6603 23.6849 0.4235 0 0.4583 0 0 3 14 35.4529 7.7118 0.704425.2688 0.3434 0 0.5417 0 0 3 15 35.3735 4.4028 0.7249 26.002 0.3536 00.625 0 0 3 16 2.2186 2.1022 0.0059 0.2132 −0.0054 0 0 0 0 4 1 27.79392.0527 0.618 22.1679 0.2794 0 0 0.125 0 4 2 28.7345 6.1964 0.591 21.20040.2887 0 0 0.1964 0 4 3 30.3974 4.4338 0.6781 24.3227 0.2923 0 0 0.26790 4 4 30.8476 10.9069 0.6382 22.8913 0.2878 0 0 0.3393 0 4 5 30.67576.3734 0.7218 25.8911 0.2804 0 0 0.4107 0 4 6 32.9835 8.0351 0.719825.8179 0.3086 0 0 0.4821 0 4 7 35.2867 7.3641 0.6966 24.9863 0.3575 0 00.5536 0 4 8 37.1287 3.7413 0.7004 25.1237 0.3921 0 0 0.625 0 4 936.5671 2.466 0.7133 25.5863 0.3845 0 0.125 0 0 4 10 35.6761 6.06190.6991 25.0759 0.3652 0 0.2083 0 0 4 11 34.9428 6.2846 0.7942 28.48740.3268 0 0.2917 0 0 4 12 37.1032 1.9047 0.7067 25.3505 0.3882 0 0.375 00 4 13 34.4347 8.2312 0.7447 26.7117 0.324 0 0.4583 0 0 4 14 34.2079.192 0.7779 27.9022 0.3061 0 0.5417 0 0 4 15 33.6393 6.2152 0.73326.2937 0.3276 0 0.625 0 0 4 16 29.037 2.5062 0.7589 27.2208 0.22490.1275 0 0 0 5 1 24.6087 9.2263 0.6037 21.6552 0.2131 0 0 0.125 0 5 224.4075 6.9158 0.6723 24.1157 0.2 0 0 0.1964 0 5 3 24.7587 11.57480.6582 23.6105 0.192 0 0 0.2679 0 5 4 26.0583 10.8227 0.7272 26.08390.2021 0 0 0.3393 0 5 5 26.7883 11.4538 0.7439 26.684 0.2078 0 0 0.41070 5 6 29.7276 12.1832 0.6912 24.7934 0.2622 0 0 0.4821 0 5 7 32.39898.3866 0.736 26.4015 0.299 0 0 0.5536 0 5 8 35.6774 6.061 0.7044 25.26780.3669 0 0 0.625 0 5 9 32.3798 8.4298 0.7432 26.6599 0.2933 0 0.125 0 05 10 31.9094 −3.0193 0.8329 29.8765 0.2864 0 0.2083 0 0 5 11 30.444711.1084 0.7665 27.4944 0.2561 0 0.2917 0 0 5 12 31.9944 9.2381 0.780928.012 0.2744 0 0.375 0 0 5 13 30.7158 12.7032 0.7995 28.6788 0.2396 00.4583 0 0 5 14 31.2335 10.2373 0.7458 26.7508 0.2628 0 0.5417 0 0 5 1529.6651 11.0649 0.8412 30.176 0.2256 0 0.625 0 0 5 16 2.021 2.859 0.02410.8632 0.0025 0 0 0 0 6 1 21.9959 11.5419 0.6402 22.9643 0.1567 0 00.125 0 6 2 23.2401 11.6565 0.6519 23.3824 0.1671 0 0 0.1964 0 6 323.4456 10.5787 0.6472 23.2142 0.1684 0 0 0.2679 0 6 4 24.307 12.70230.699 25.0731 0.1689 0 0 0.3393 0 6 5 25.1127 14.8654 0.7048 25.28010.1705 0 0 0.4107 0 6 6 27.3528 15.4064 0.695 24.9286 0.2121 0 0 0.48210 6 7 27.7231 13.6272 0.7298 26.1773 0.2096 0 0 0.5536 0 6 8 30.918312.3963 0.7109 25.5005 0.2709 0 0 0.625 0 6 9 31.5914 9.2633 0.809929.0513 0.2665 0 0.125 0 0 6 10 28.5927 14.8272 0.7457 26.7502 0.218 00.2083 0 0 6 11 29.3514 14.8513 0.757 27.1537 0.2308 0 0.2917 0 0 6 1228.9816 17.4189 0.7629 27.3641 0.2128 0 0.375 0 0 6 13 28.941 15.91950.838 30.0593 0.1974 0 0.4583 0 0 6 14 27.4163 18.9987 0.7599 27.25850.203 0 0.5417 0 0 6 15 28.7449 11.147 0.819 29.378 0.2121 0 0.625 0 0 616 0.9839 1.6606 −0.0142 −0.5093 −0.004 0 0 0 0 7 1 18.9135 12.94120.6042 21.6717 0.1144 0 0 0.125 0 7 2 20.7984 12.6454 0.6392 22.92690.1259 0 0 0.1964 0 7 3 21.3309 14.0442 0.6719 24.1021 0.1203 0 0 0.26790 7 4 23.3179 12.6244 0.7101 25.4707 0.1495 0 0 0.3393 0 7 5 22.31115.9169 0.6986 25.0598 0.1228 0 0 0.4107 0 7 6 24.9395 15.9225 0.71725.7205 0.1568 0 0 0.4821 0 7 7 27.218 13.6346 0.757 27.1547 0.194 0 00.5536 0 7 8 29.1374 13.3752 0.7671 27.5172 0.223 0 0 0.625 0 7 927.2823 14.9173 0.7823 28.0598 0.18 0 0.125 0 0 7 10 26.7129 17.03880.7718 27.6846 0.1641 0 0.2083 0 0 7 11 27.8928 14.018 0.8136 29.18320.1802 0 0.2917 0 0 7 12 27.6216 14.289 0.8323 29.8536 0.171 0 0.375 0 07 13 27.1789 15.5566 0.8155 29.2535 0.1736 0 0.4583 0 0 7 14 26.957615.5396 0.8192 29.3865 0.1669 0 0.5417 0 0 7 15 26.8378 18.0959 0.804328.8522 0.1535 0 0.625 0 0 7 16 0.8467 −0.7636 −0.0188 −0.6755 0.0049 00 0 0 8 1 19.7963 10.1989 0.6673 23.9369 0.121 0 0 0.125 0 8 2 21.044112.1292 0.6771 24.2868 0.1148 0 0 0.1964 0 8 3 21.5826 10.3589 0.716525.7009 0.1225 0 0 0.2679 0 8 4 22.5419 11.3314 0.748 26.8328 0.1302 0 00.3393 0 8 5 21.6915 15.8069 0.7002 25.1158 0.1194 0 0 0.4107 0 8 623.1549 15.2824 0.7452 26.7299 0.134 0 0 0.4821 0 8 7 25.5149 14.2440.7133 25.5881 0.1741 0 0 0.5536 0 8 8 30.5353 11.7823 0.7776 27.89420.2489 0 0 0.625 0 8 9 27.3885 11.511 0.828 29.7013 0.1795 0 0.125 0 0 810 25.7173 17.922 0.7754 27.8131 0.1478 0 0.2083 0 0 8 11 26.414413.4264 0.8202 29.4217 0.1633 0 0.2917 0 0 8 12 27.705 13.0097 0.886631.8026 0.1641 0 0.375 0 0 8 13 25.995 17.4887 0.7963 28.5649 0.1547 00.4583 0 0 8 14 26.4681 16.9554 0.79 28.3384 0.1536 0 0.5417 0 0 8 1526.4678 13.3955 0.8162 29.2769 0.159 0 0.625 0 0 8 16 0.9966 1.4271−0.0301 1.0794 0.001 0 0 0 0 9 1 31.9347 0.0878 0.5856 21.005 0.3559 0 00 0.125 9 2 31.1011 4.4646 0.6363 22.8244 0.313 0 0 0 0.2083 9 3 30.30855.038 0.6449 23.1338 0.292 0 0 0 0.2917 9 4 34.5542 −0.385 0.642823.0592 0.3696 0 0 0 0.375 9 5 32.8174 2.5843 0.688 24.6778 0.3271 0 0 00.4583 9 6 33.2672 3.4632 0.7089 25.4293 0.3193 0 0 0 0.5417 9 7 33.34066.7818 0.7546 27.0667 0.3065 0 0 0 0.625 9 8 30.1425 10.1464 0.806828.94 0.2311 0.1275 0 0 0 9 9 26.7465 13.6126 0.797 28.5881 0.1718 00.125 0 0 9 10 25.7719 14.0036 0.7994 28.6761 0.1518 0 0.2083 0 0 9 1126.5309 12.4669 0.8451 30.3128 0.1559 0 0.2917 0 0 9 12 25.9916 18.14070.7856 28.1815 0.1412 0 0.375 0 0 9 13 27.5347 12.2179 0.8823 31.650.1621 0 0.4583 0 0 9 14 27.449 13.4272 0.8785 31.514 0.1596 0 0.5417 00 9 15 27.2031 12.7934 0.8659 31.0587 0.16 0 0.625 0 0 9 16 1.42630.8064 −0.0206 −0.738 −0.008 0 0 0 0 10 1 32.3674 −1.4914 0.5724 20.5340.364 0 0 0 0.125 10 2 29.9213 4.6079 0.6504 23.3302 0.2906 0 0 0 0.208310 3 31.2861 3.8032 0.6813 24.4397 0.2991 0 0 0 0.2917 10 4 30.38736.0311 0.7192 25.7991 0.267 0 0 0 0.375 10 5 28.9002 6.7708 0.720425.841 0.2411 0 0 0 0.4583 10 6 32.0239 4.8199 0.6949 24.9252 0.3029 0 00 0.5417 10 7 30.5572 5.6388 0.7245 25.9878 0.2706 0 0 0 0.625 10 840.4396 −5.5116 0.616 22.0945 0.4779 0 0 0 0 10 9 36.6242 −0.3514 0.686124.6123 0.3891 0 0 0 0 10 10 36.4527 2.4838 0.6743 24.1867 0.3709 0 0 00 10 11 41.5385 −5.8909 0.5621 20.1619 0.4989 0 0 0 0 10 12 40.6949−2.4705 0.5969 21.4112 0.4762 0 0 0 0 10 13 42.2576 −5.7126 0.557620.0014 0.5199 0 0 0 0 10 14 41.6714 −3.6275 0.5605 20.1036 0.5139 0 0 00 10 15 42.1852 −8.2409 0.5642 20.2385 0.5399 0 0 0 0 10 16 29.060811.8827 0.7591 27.2282 0.2128 0.1275 0 0 0 11 1 28.5929 −0.5506 0.621122.279 0.2956 0 0 0 0.125 11 2 29.7686 2.427 0.6583 23.6124 0.3009 0 0 00.2083 11 3 27.9031 6.2226 0.7105 25.4845 0.2357 0 0 0 0.2917 11 427.7859 5.6743 0.7722 27.6991 0.2233 0 0 0 0.375 11 5 28.1184 7.27720.7741 27.7691 0.2183 0 0 0 0.4583 11 6 29.7411 6.3505 0.739 26.50980.2566 0 0 0 0.5417 11 7 28.9209 10.6911 0.7589 27.2215 0.2176 0 0 00.625 11 8 38.2687 −0.4875 0.6363 22.8233 0.4263 0 0 0 0 11 9 36.09721.1534 0.6782 24.3267 0.3858 0 0 0 0 11 10 37.1677 0.2763 0.6847 24.56060.3885 0 0 0 0 11 11 36.4236 −0.1779 0.7178 25.7481 0.3764 0 0 0 0 11 1236.1786 1.7764 0.7141 25.6149 0.3717 0 0 0 0 11 13 36.8922 0.6262 0.731726.2452 0.3798 0 0 0 0 11 14 37.7602 −1.1368 0.6728 24.133 0.4075 0 0 00 11 15 37.5647 0.0323 0.6314 22.6471 0.4137 0 0 0 0 11 16 2.1619−0.4379 0.0003 0.0124 0.0018 0 0 0 0 12 1 26.4704 3.8573 0.6373 22.86180.244 0 0 0 0.125 12 2 25.123 8.1044 0.6894 24.7289 0.1974 0 0 0 0.208312 3 25.0006 11.6691 0.6754 24.2266 0.1793 0 0 0 0.2917 12 4 25.74969.018 0.7275 26.094 0.1858 0 0 0 0.375 12 5 26.83 9.6173 0.7402 26.55070.1975 0 0 0 0.4583 12 6 27.8818 9.0527 0.7288 26.1427 0.2213 0 0 00.5417 12 7 27.1932 8.8863 0.7352 26.3714 0.2004 0 0 0 0.625 12 833.3109 4.6111 0.6956 24.952 0.3233 0 0 0 0 12 9 34.2433 1.3375 0.687424.657 0.3411 0 0 0 0 12 10 33.5455 4.5252 0.6868 24.6346 0.3233 0 0 0 012 11 33.7382 2.6662 0.6856 24.5945 0.3378 0 0 0 0 12 12 32.2421 4.41520.7066 25.3444 0.3056 0 0 0 0 12 13 32.1276 4.4582 0.7235 25.9518 0.29310 0 0 0 12 14 33.6765 4.2381 0.6886 24.6996 0.3353 0 0 0 0 12 15 32.80471.0222 0.6672 23.9322 0.335 0 0 0 0 12 16 0.201 −6.0934 −0.0375 −1.3439−0.0082 0 0 0 0 13 1 23.6285 7.246 0.6392 22.9288 0.1884 0 0 0 0.125 132 24.886 9.7562 0.7072 25.3683 0.1859 0 0 0 0.2083 13 3 24.8624 12.42650.6961 24.9691 0.1723 0 0 0 0.2917 13 4 24.9826 10.6722 0.7365 26.41710.1754 0 0 0 0.375 13 5 25.7305 12.1843 0.7732 27.7354 0.1708 0 0 00.4583 13 6 25.6747 13.2113 0.7366 26.4231 0.1687 0 0 0 0.5417 13 726.0976 11.7018 0.7694 27.5973 0.172 0 0 0 0.625 13 8 30.4445 8.59990.7335 26.3099 0.2569 0 0 0 0 13 9 30.2838 9.6966 0.7263 26.0542 0.25490 0 0 0 13 10 30.4598 8.76 0.7709 27.6538 0.2542 0 0 0 0 13 11 30.34139.6956 0.7293 26.1594 0.2487 0 0 0 0 13 12 30.4805 9.6042 0.7384 26.4870.2567 0 0 0 0 13 13 30.7866 8.4894 0.7264 26.0577 0.2594 0 0 0 0 13 1430.0474 8.3188 0.7452 26.7323 0.2523 0 0 0 0 13 15 29.1492 8.7192 0.72225.9001 0.2422 0 0 0 0 13 16 0.1828 −0.1024 −0.0281 −1.0092 −0.0071 0 00 0 14 1 22.2722 8.7244 0.645 23.1379 0.1695 0 0 0 0.125 14 2 22.523410.8931 0.7013 25.1544 0.1529 0 0 0 0.2083 14 3 23.2966 10.4674 0.7326.1842 0.1515 0 0 0 0.2917 14 4 23.0657 11.1311 0.7205 25.8432 0.1445 00 0 0.375 14 5 23.5149 10.9662 0.7361 26.4053 0.1454 0 0 0 0.4583 14 624.2862 10.9726 0.7503 26.9142 0.1569 0 0 0 0.5417 14 7 24.5053 10.88210.7621 27.3379 0.1507 0 0 0 0.625 14 8 27.3028 9.2784 0.6918 24.81370.2118 0 0 0 0 14 9 27.5076 9.6923 0.7089 25.4269 0.2149 0 0 0 0 14 1028.334 9.5711 0.7353 26.3752 0.2233 0 0 0 0 14 11 27.0996 10.2648 0.705225.2943 0.205 0 0 0 0 14 12 27.44 10.2454 0.7478 26.8252 0.2075 0 0 0 014 13 27.1174 10.8853 0.7218 25.8925 0.1998 0 0 0 0 14 14 27.7049 8.97470.7326 26.2773 0.2161 0 0 0 0 14 15 26.6173 9.1156 0.7031 25.2221 0.20440 0 0 0 14 16 0.0041 −1.9313 0.0371 1.3316 0.0149 0 0 0 0 15 1 21.33277.9702 0.6812 24.4361 0.1457 0 0 0 0.125 15 2 22.5406 10.7433 0.694124.897 0.164 0 0 0 0.2083 15 3 23.3395 12.6857 0.7286 26.1338 0.1508 0 00 0.2917 15 4 22.5094 11.0489 0.6988 25.0645 0.1555 0 0 0 0.375 15 524.0319 11.5771 0.7533 27.0223 0.1559 0 0 0 0.4583 15 6 23.7127 13.44410.7425 26.6323 0.1473 0 0 0 0.5417 15 7 23.9044 13.6139 0.74 26.54310.1463 0 0 0 0.625 15 8 27.3093 8.6187 0.6879 24.6757 0.2267 0 0 0 0 159 25.8606 9.1289 0.6874 24.6566 0.2042 0 0 0 0 15 10 27.5146 9.5420.7239 25.968 0.2143 0 0 0 0 15 11 26.8709 11.7285 0.7185 25.7726 0.19280 0 0 0 15 12 27.18 9.7353 0.7526 26.9952 0.2076 0 0 0 0 15 13 26.135511.7091 0.7385 26.4915 0.193 0 0 0 0 15 14 26.448 10.1089 0.7389 26.5040.1951 0 0 0 0 15 15 25.0723 11.1257 0.717 25.7198 0.1817 0 0 0 0 15 160.1716 0.3824 −0.0242 −0.8681 −0.0157 0 0 0 0 16 1 18.4383 9.1302 0.599921.5188 0.1141 0 0 0 0.125 16 2 19.8583 4.0253 0.4578 16.4203 0.1998 0 00 0.2083 16 3 19.5944 4.9317 0.4823 17.2995 0.1854 0 0 0 0.2917 16 420.6005 6.4056 0.535 19.1892 0.1902 0 0 0 0.375 16 5 20.7488 9.22720.6225 22.3294 0.16 0 0 0 0.4583 16 6 22.0224 9.9861 0.696 24.96470.1575 0 0 0 0.5417 16 7 22.6337 10.2429 0.6902 24.7569 0.1565 0 0 00.625 16 8 25.0532 7.0189 0.6701 24.0379 0.2148 0 0 0 0 16 9 24.72996.5606 0.6124 21.9688 0.2183 0 0 0 0 16 10 24.7277 6.8082 0.5753 20.63490.2229 0 0 0 0 16 11 24.3287 6.2367 0.5779 20.7309 0.22 0 0 0 0 16 1223.4654 5.4951 0.5533 19.8459 0.2196 0 0 0 0 16 13 24.6899 6.4164 0.620322.2522 0.2161 0 0 0 0 16 14 23.6155 3.836 0.5379 19.2945 0.2324 0 0 0 016 15 22.1905 5.0337 0.5364 19.2395 0.212 0 0 0 0 16 16 27.2507 9.6040.8059 28.9067 0.2014 0.1275 0 0 0 Tem- pera- ture: PtNH32NO22 300 C.(unsta- SUM_(—) mol % mol % mol % mol % mol % mol % R C bilized)RuNONO33 ZrONO32 micromols C Co La Pt Ru Zr real real real real real 1 10 0 0 0.1275 0 0 0 100 0 0 1 2 0 0 0 0 0 0 0 0 0 0 1 3 0 0 0 0 0 0 0 0 00 1 4 0 0 0 0 0 0 0 0 0 0 1 5 0 0 0 0 0 0 0 0 0 0 1 6 0 0 0 0 0 0 0 0 00 1 7 0 0 0 0.1275 0 0 0 100 0 0 1 8 0 0 0 0 0 0 0 0 0 0 1 9 0 0 0 0 0 00 0 0 0 1 10 0 0 0 0 0 0 0 0 0 0 1 11 0 0 0 0 0 0 0 0 0 0 1 12 0 0 0 0 00 0 0 0 0 1 13 0 0 0 0.1275 0 0 0 100 0 0 1 14 0 0 0 0 0 0 0 0 0 0 1 150 0 0 0 0 0 0 0 0 0 1 16 0 0 0 0 0 0 0 0 0 0 2 1 0.1275 0.0618 0 0.31430 39.77 0 40.56 19.67 0 2 2 0.1275 0.0618 0 0.3857 0 50.92 0 33.05 16.020 2 3 0.1275 0.0618 0 0.4572 0 58.59 0 27.89 13.52 0 2 4 0.1275 0.0618 00.5286 0 64.19 0 24.12 11.69 0 2 5 0.1275 0.0618 0 0.6 0 68.45 0 21.2510.3 0 2 6 0.1275 0.0618 0 0.6715 0 71.81 0 18.99 9.21 0 2 7 0.12750.0618 0 0.7429 0 74.52 0 17.16 8.32 0 2 8 0.1275 0.0618 0 0.8143 076.75 0 15.66 7.59 0 2 9 0.1275 0.0618 0 0.3143 39.77 0 0 40.56 19.67 02 10 0.1275 0.0618 0 0.3976 52.39 0 0 32.06 15.54 0 2 11 0.1275 0.0618 00.481 60.64 0 0 26.51 12.85 0 2 12 0.1275 0.0618 0 0.5643 66.45 0 022.59 10.95 0 2 13 0.1275 0.0618 0 0.6476 70.77 0 0 19.69 9.54 0 2 140.1275 0.0618 0 0.731 74.1 0 0 17.44 8.46 0 2 15 0.1275 0.0618 0 0.814376.75 0 0 15.66 7.59 0 2 16 0 0 0 0 0 0 0 0 0 0 3 1 0.1275 0.0536 00.3061 0 40.84 0 41.66 17.5 0 3 2 0.1275 0.0536 0 0.3775 0 52.03 0 33.7714.19 0 3 3 0.1275 0.0536 0 0.4489 0 59.67 0 28.4 11.93 0 3 4 0.12750.0536 0 0.5204 0 65.2 0 24.5 10.3 0 3 5 0.1275 0.0536 0 0.5918 0 69.4 021.54 9.05 0 3 6 0.1275 0.0536 0 0.6632 0 72.7 0 19.22 8.08 0 3 7 0.12750.0536 0 0.7346 0 75.35 0 17.36 7.29 0 3 8 0.1275 0.0536 0 0.8061 077.54 0 15.82 6.65 0 3 9 0.1275 0.0547 0 0.3072 40.68 0 0 41.5 17.82 0 310 0.1275 0.0547 0 0.3906 53.34 0 0 32.64 14.02 0 3 11 0.1275 0.0547 00.4739 61.54 0 0 26.9 11.55 0 3 12 0.1275 0.0547 0 0.5572 67.29 0 022.88 9.82 0 3 13 0.1275 0.0547 0 0.6406 71.55 0 0 19.9 8.55 0 3 140.1275 0.0547 0 0.7239 74.82 0 0 17.61 7.56 0 3 15 0.1275 0.0547 00.8072 77.42 0 0 15.79 6.78 0 3 16 0 0 0 0 0 0 0 0 0 0 4 1 0.1275 0.04530 0.2978 0 41.97 0 42.81 15.22 0 4 2 0.1275 0.0453 0 0.3693 0 53.2 034.53 12.28 0 4 3 0.1275 0.0453 0 0.4407 0 60.78 0 28.93 10.29 0 4 40.1275 0.0453 0 0.5121 0 66.25 0 24.9 8.85 0 4 5 0.1275 0.0453 0 0.58350 70.38 0 21.85 7.77 0 4 6 0.1275 0.0453 0 0.655 0 73.61 0 19.47 6.92 04 7 0.1275 0.0453 0 0.7264 0 76.21 0 17.55 6.24 0 4 8 0.1275 0.0453 00.7978 0 78.34 0 15.98 5.68 0 4 9 0.1275 0.0477 0 0.3002 41.64 0 0 42.4715.88 0 4 10 0.1275 0.0477 0 0.3835 54.32 0 0 33.24 12.43 0 4 11 0.12750.0477 0 0.4669 62.48 0 0 27.31 10.21 0 4 12 0.1275 0.0477 0 0.550268.16 0 0 23.17 8.67 0 4 13 0.1275 0.0477 0 0.6335 72.35 0 0 20.13 7.530 4 14 0.1275 0.0477 0 0.7169 75.56 0 0 17.79 6.65 0 4 15 0.1275 0.04770 0.8002 78.11 0 0 15.93 5.96 0 4 16 0 0 0 0.1275 0 0 0 100 0 0 5 10.1275 0.0371 0 0.2896 0 43.16 0 44.03 12.81 0 5 2 0.1275 0.0371 0 0.3610 54.41 0 35.32 10.27 0 5 3 0.1275 0.0371 0 0.4324 0 61.94 0 29.48 8.580 5 4 0.1275 0.0371 0 0.5039 0 67.34 0 25.3 7.36 0 5 5 0.1275 0.0371 00.5753 0 71.39 0 22.16 6.45 0 5 6 0.1275 0.0371 0 0.6467 0 74.55 0 19.715.73 0 5 7 0.1275 0.0371 0 0.7182 0 77.08 0 17.75 5.16 0 5 8 0.12750.0371 0 0.7896 0 79.16 0 16.15 4.7 0 5 9 0.1275 0.0406 0 0.2931 42.64 00 43.5 13.86 0 5 10 0.1275 0.0406 0 0.3765 55.34 0 0 33.87 10.79 0 5 110.1275 0.0406 0 0.4598 63.44 0 0 27.73 8.83 0 5 12 0.1275 0.0406 00.5431 69.05 0 0 23.48 7.48 0 5 13 0.1275 0.0406 0 0.6265 73.16 0 020.35 6.48 0 5 14 0.1275 0.0406 0 0.7098 76.31 0 0 17.96 5.72 0 5 150.1275 0.0406 0 0.7931 78.8 0 0 16.08 5.12 0 5 16 0 0 0 0 0 0 0 0 0 0 61 0.1275 0.0288 0 0.2813 0 44.43 0 45.32 10.25 0 6 2 0.1275 0.0288 00.3528 0 55.68 0 36.14 8.18 0 6 3 0.1275 0.0288 0 0.4242 0 63.14 0 30.066.8 0 6 4 0.1275 0.0288 0 0.4956 0 68.46 0 25.72 5.82 0 6 5 0.12750.0288 0 0.5671 0 72.43 0 22.48 5.09 0 6 6 0.1275 0.0288 0 0.6385 075.51 0 19.97 4.52 0 6 7 0.1275 0.0288 0 0.7099 0 77.98 0 17.96 4.06 0 68 0.1275 0.0288 0 0.7813 0 79.99 0 16.32 3.69 0 6 9 0.1275 0.0336 00.2861 43.7 0 0 44.57 11.73 0 6 10 0.1275 0.0336 0 0.3694 56.4 0 0 34.529.08 0 6 11 0.1275 0.0336 0 0.4527 64.43 0 0 28.16 7.41 0 6 12 0.12750.0336 0 0.5361 69.96 0 0 23.78 6.26 0 6 13 0.1275 0.0336 0 0.6194 74 00 20.58 5.42 0 6 14 0.1275 0.0336 0 0.7027 77.08 0 0 18.14 4.78 0 6 150.1275 0.0336 0 0.7861 79.51 0 0 16.22 4.27 0 6 16 0 0 0 0 0 0 0 0 0 0 71 0.1275 0.0206 0 0.2731 0 45.77 0 46.69 7.54 0 7 2 0.1275 0.0206 00.3445 0 57.01 0 37.01 5.98 0 7 3 0.1275 0.0206 0 0.416 0 64.39 0 30.654.95 0 7 4 0.1275 0.0206 0 0.4874 0 69.61 0 26.16 4.23 0 7 5 0.12750.0206 0 0.5588 0 73.5 0 22.82 3.69 0 7 6 0.1275 0.0206 0 0.6302 0 76.50 20.23 3.27 0 7 7 0.1275 0.0206 0 0.7017 0 78.89 0 18.17 2.94 0 7 80.1275 0.0206 0 0.7731 0 80.84 0 16.49 2.67 0 7 9 0.1275 0.0265 0 0.27944.8 0 0 45.7 9.5 0 7 10 0.1275 0.0265 0 0.3623 57.5 0 0 35.19 7.31 0 711 0.1275 0.0265 0 0.4457 65.45 0 0 28.61 5.94 0 7 12 0.1275 0.0265 00.529 70.89 0 0 24.1 5.01 0 7 13 0.1275 0.0265 0 0.6123 74.85 0 0 20.824.33 0 7 14 0.1275 0.0265 0 0.6957 77.86 0 0 18.33 3.81 0 7 15 0.12750.0265 0 0.779 80.23 0 0 16.37 3.4 0 7 16 0 0 0 0 0 0 0 0 0 0 8 1 0.12750.0124 0 0.2649 0 47.19 0 48.14 4.67 0 8 2 0.1275 0.0124 0 0.3363 058.41 0 37.91 3.68 0 8 3 0.1275 0.0124 0 0.4077 0 65.7 0 31.27 3.03 0 84 0.1275 0.0124 0 0.4791 0 70.81 0 26.61 2.58 0 8 5 0.1275 0.0124 00.5506 0 74.6 0 23.16 2.25 0 8 6 0.1275 0.0124 0 0.622 0 77.51 0 20.51.99 0 8 7 0.1275 0.0124 0 0.6934 0 79.83 0 18.39 1.78 0 8 8 0.12750.0124 0 0.7649 0 81.71 0 16.67 1.62 0 8 9 0.1275 0.0194 0 0.2719 45.970 0 46.89 7.14 0 8 10 0.1275 0.0194 0 0.3553 58.64 0 0 35.89 5.47 0 8 110.1275 0.0194 0 0.4386 66.5 0 0 29.07 4.43 0 8 12 0.1275 0.0194 0 0.521971.85 0 0 24.43 3.72 0 8 13 0.1275 0.0194 0 0.6053 75.73 0 0 21.07 3.210 8 14 0.1275 0.0194 0 0.6886 78.66 0 0 18.52 2.82 0 8 15 0.1275 0.01940 0.7719 80.97 0 0 16.52 2.52 0 8 16 0 0 0 0 0 0 0 0 0 0 9 1 0.12750.0618 0 0.3143 0 0 39.77 40.56 19.67 0 9 2 0.1275 0.0618 0 0.3976 0 052.39 32.06 15.54 0 9 3 0.1275 0.0618 0 0.481 0 0 60.64 26.51 12.85 0 94 0.1275 0.0618 0 0.5643 0 0 66.45 22.59 10.95 0 9 5 0.1275 0.0618 00.6476 0 0 70.77 19.69 9.54 0 9 6 0.1275 0.0618 0 0.731 0 0 74.1 17.448.46 0 9 7 0.1275 0.0618 0 0.8143 0 0 76.75 15.66 7.59 0 9 8 0 0 00.1275 0 0 0 100 0 0 9 9 0.1275 0.0124 0 0.2649 47.19 0 0 48.14 4.67 0 910 0.1275 0.0124 0 0.3482 59.83 0 0 36.62 3.55 0 9 11 0.1275 0.0124 00.4315 67.59 0 0 29.55 2.86 0 9 12 0.1275 0.0124 0 0.5149 72.83 0 024.76 2.4 0 9 13 0.1275 0.0124 0 0.5982 76.62 0 0 21.31 2.07 0 9 140.1275 0.0124 0 0.6815 79.48 0 0 18.71 1.81 0 9 15 0.1275 0.0124 00.7649 81.71 0 0 16.67 1.62 0 9 16 0 0 0 0 0 0 0 0 0 0 10 1 0.12750.0547 0 0.3072 0 0 40.68 41.5 17.82 0 10 2 0.1275 0.0547 0 0.3906 0 053.34 32.64 14.02 0 10 3 0.1275 0.0547 0 0.4739 0 0 61.54 26.9 11.55 010 4 0.1275 0.0547 0 0.5572 0 0 67.29 22.88 9.82 0 10 5 0.1275 0.0547 00.6406 0 0 71.55 19.9 8.55 0 10 6 0.1275 0.0547 0 0.7239 0 0 74.82 17.617.56 0 10 7 0.1275 0.0547 0 0.8072 0 0 77.42 15.79 6.78 0 10 8 0.12750.0618 0.125 0.3143 0 0 0 40.56 19.67 39.77 10 9 0.1275 0.0618 0.19640.3857 0 0 0 33.05 16.02 50.92 10 10 0.1275 0.0618 0.2679 0.4572 0 0 027.89 13.52 58.59 10 11 0.1275 0.0618 0.3393 0.5286 0 0 0 24.12 11.6964.19 10 12 0.1275 0.0618 0.4107 0.6 0 0 0 21.25 10.3 68.45 10 13 0.12750.0618 0.4821 0.6715 0 0 0 18.99 9.21 71.81 10 14 0.1275 0.0618 0.55360.7429 0 0 0 17.16 8.32 74.52 10 15 0.1275 0.0618 0.625 0.8143 0 0 015.66 7.59 76.75 10 16 0 0 0 0.1275 0 0 0 100 0 0 11 1 0.1275 0.0477 00.3002 0 0 41.64 42.47 15.88 0 11 2 0.1275 0.0477 0 0.3835 0 0 54.3233.24 12.43 0 11 3 0.1275 0.0477 0 0.4669 0 0 62.48 27.31 10.21 0 11 40.1275 0.0477 0 0.5502 0 0 68.16 23.17 8.67 0 11 5 0.1275 0.0477 00.6335 0 0 72.35 20.13 7.53 0 11 6 0.1275 0.0477 0 0.7169 0 0 75.5617.79 6.65 0 11 7 0.1275 0.0477 0 0.8002 0 0 78.11 15.93 5.96 0 11 80.1275 0.0536 0.125 0.3061 0 0 0 41.66 17.5 40.84 11 9 0.1275 0.05360.1964 0.3775 0 0 0 33.77 14.19 52.03 11 10 0.1275 0.0536 0.2679 0.44890 0 0 28.4 11.93 59.67 11 11 0.1275 0.0536 0.3393 0.5204 0 0 0 24.5 10.365.2 11 12 0.1275 0.0536 0.4107 0.5918 0 0 0 21.54 9.05 69.4 11 130.1275 0.0536 0.4821 0.6632 0 0 0 19.22 8.08 72.7 11 14 0.1275 0.05360.5536 0.7346 0 0 0 17.36 7.29 75.35 11 15 0.1275 0.0536 0.625 0.8061 00 0 15.82 6.65 77.54 11 16 0 0 0 0 0 0 0 0 0 0 12 1 0.1275 0.0406 00.2931 0 0 42.64 43.5 13.86 0 12 2 0.1275 0.0406 0 0.3765 0 0 55.3433.87 10.79 0 12 3 0.1275 0.0406 0 0.4598 0 0 63.44 27.73 8.83 0 12 40.1275 0.0406 0 0.5431 0 0 69.05 23.48 7.48 0 12 5 0.1275 0.0406 00.6265 0 0 73.16 20.35 6.48 0 12 6 0.1275 0.0406 0 0.7098 0 0 76.3117.96 5.72 0 12 7 0.1275 0.0406 0 0.7931 0 0 78.8 16.08 5.12 0 12 80.1275 0.0453 0.125 0.2978 0 0 0 42.81 15.22 41.97 12 9 0.1275 0.04530.1964 0.3693 0 0 0 34.53 12.28 53.2 12 10 0.1275 0.0453 0.2679 0.4407 00 0 28.93 10.29 60.78 12 11 0.1275 0.0453 0.3393 0.5121 0 0 0 24.9 8.8566.25 12 12 0.1275 0.0453 0.4107 0.5835 0 0 0 21.85 7.77 70.38 12 130.1275 0.0453 0.4821 0.655 0 0 0 19.47 6.92 73.61 12 14 0.1275 0.04530.5536 0.7264 0 0 0 17.55 6.24 76.21 12 15 0.1275 0.0453 0.625 0.7978 00 0 15.98 5.68 78.34 12 16 0 0 0 0 0 0 0 0 0 0 13 1 0.1275 0.0336 00.2861 0 0 43.7 44.57 11.73 0 13 2 0.1275 0.0336 0 0.3694 0 0 56.4 34.529.08 0 13 3 0.1275 0.0336 0 0.4527 0 0 64.43 28.16 7.41 0 13 4 0.12750.0336 0 0.5361 0 0 69.96 23.78 6.26 0 13 5 0.1275 0.0336 0 0.6194 0 074 20.58 5.42 0 13 6 0.1275 0.0336 0 0.7027 0 0 77.08 18.14 4.78 0 13 70.1275 0.0336 0 0.7861 0 0 79.510939 28 16.22 4.27 0 13 8 0.1275 0.03710.125 0.2896 0 0 0 44.03 12.81 43.16 13 9 0.1275 0.0371 0.1964 0.361 0 00 35.32 10.27 54.41 13 10 0.1275 0.0371 0.2679 0.4324 0 0 0 29.48 8.5861.94 13 11 0.1275 0.0371 0.3393 0.5039 0 0 0 25.3 7.36 67.34 13 120.1275 0.0371 0.4107 0.5753 0 0 0 22.16 6.45 71.39 13 13 0.1275 0.03710.4821 0.6467 0 0 0 19.71 5.73 74.55 13 14 0.1275 0.0371 0.5536 0.7182 00 0 17.75 5.16 77.08 13 15 0.1275 0.0371 0.625 0.7896 0 0 0 16.15 4.779.16 13 16 0 0 0 0 0 0 0 0 0 0 14 1 0.1275 0.0265 0 0.279 0 0 44.8 45.79.5 0 14 2 0.1275 0.0265 0 0.3623 0 0 57.5 35.19 7.31 0 14 3 0.12750.0265 0 0.4457 0 0 65.45 28.61 5.94 0 14 4 0.1275 0.0265 0 0.529 0 070.89 24.1 5.01 0 14 5 0.1275 0.0265 0 0.6123 0 0 74.85 20.82 4.33 0 146 0.1275 0.0265 0 0.6957 0 0 77.86 18.33 3.81 0 14 7 0.1275 0.0265 00.779 0 0 80.23 16.37 3.4 0 14 8 0.1275 0.0288 0.125 0.2813 0 0 0 45.3210.25 44.43 14 9 0.1275 0.0288 0.1964 0.3528 0 0 0 36.14 8.18 55.68 1410 0.1275 0.0288 0.2679 0.4242 0 0 0 30.06 6.8 63.14 14 11 0.1275 0.02880.3393 0.4956 0 0 0 25.72 5.82 68.46 14 12 0.1275 0.0288 0.4107 0.5671 00 0 22.48 5.09 72.43 14 13 0.1275 0.0288 0.4821 0.6385 0 0 0 19.97 4.5275.51 14 14 0.1275 0.0288 0.5536 0.7099 0 0 0 17.96 4.06 77.98 14 150.1275 0.0288 0.625 0.7813 0 0 0 16.32 3.69 79.99 14 16 0 0 0 0 0 0 0 00 0 15 1 0.1275 0.0194 0 0.2719 0 0 45.97 46.89 7.14 0 15 2 0.12750.0194 0 0.3553 0 0 58.64 35.89 5.47 0 15 3 0.1275 0.0194 0 0.4386 0 066.5 29.07 4.43 0 15 4 0.1275 0.0194 0 0.5219 0 0 71.85 24.43 3.72 0 155 0.1275 0.0194 0 0.6053 0 0 75.73 21.07 3.21 0 15 6 0.1275 0.0194 00.6886 0 0 78.66 18.52 2.82 0 15 7 0.1275 0.0194 0 0.7719 0 0 80.9716.52 2.52 0 15 8 0.1275 0.0206 0.125 0.2731 0 0 0 46.69 7.54 45.77 15 90.1275 0.0206 0.1964 0.3445 0 0 0 37.01 5.98 57.01 15 10 0.1275 0.02060.2679 0.416 0 0 0 30.65 4.95 64.39 15 11 0.1275 0.0206 0.3393 0.4874 00 0 26.16 4.23 69.61 15 12 0.1275 0.0206 0.4107 0.5588 0 0 0 22.82 3.6973.5 15 13 0.1275 0.0206 0.4821 0.6302 0 0 0 20.23 3.27 76.5 15 140.1275 0.0206 0.5536 0.7017 0 0 0 18.17 2.94 78.89 15 15 0.1275 0.02060.625 0.7731 0 0 0 16.49 2.67 80.84 15 16 0 0 0 0 0 0 0 0 0 0 16 10.1275 0.0124 0 0.2649 0 0 47.19 48.14 4.67 0 16 2 0.1275 0.0124 00.3482 0 0 59.83 36.62 3.55 0 16 3 0.1275 0.0124 0 0.4315 0 0 67.5929.55 2.86 0 16 4 0.1275 0.0124 0 0.5149 0 0 72.83 24.76 2.4 0 16 50.1275 0.0124 0 0.5982 0 0 76.62 21.31 2.07 0 16 6 0.1275 0.0124 00.6815 0 0 79.48 18.71 1.81 0 16 7 0.1275 0.0124 0 0.7649 0 0 81.7116.67 1.62 0 16 8 0.1275 0.0124 0.125 0.2649 0 0 0 48.14 4.67 47.19 16 90.1275 0.0124 0.1964 0.3363 0 0 0 37.91 3.68 58.41 16 10 0.1275 0.01240.2679 0.4077 0 0 0 31.27 3.03 65.7 16 11 0.1275 0.0124 0.3393 0.4791 00 0 26.61 2.58 70.81 16 12 0.1275 0.0124 0.4107 0.5506 0 0 0 23.16 2.2574.6 16 13 0.1275 0.0124 0.4821 0.622 0 0 0 20.5 1.99 77.51 16 14 0.12750.0124 0.5536 0.6934 0 0 0 18.39 1.78 79.83 16 15 0.1275 0.0124 0.6250.7649 0 0 0 16.67 1.62 81.71 16 16 0 0 0 0.1275 0 0 0 100 0 0

[0297] TABLE III Tem- pera- ture: 350 C. Pt1.O%/ R C COCONV H2OCONVC02PROD C02PERPROD CH4PROD ZrO2_std FeNO33 LaNO33 NH42TiOOX2 PtNH32NO22real real real real real real real real real real real real 1 1 20.74134.5453 0.4037 14.2873 0.2832 0.1275 0 0 0 0 1 2 1.0598 3.2201 0.04611.6326 0.0082 0 0 0 0 0 1 3 0.3696 3.2009 0.0209 0.7387 −0.0014 0 0 0 00 1 4 −1.0203 −0.9111 0.0365 1.2925 0.0097 0 0 0 0 0 1 5 −2.8069 −1.4712−0.0045 −0.1594 0.0035 0 0 0 0 0 1 6 1.2699 0.7698 0.0267 0.9456 −0.00250 0 0 0 0 1 7 22.8232 0.1219 0.3846 13.6114 0.2965 0.1275 0 0 0 0 1 80.4252 0.1401 0.0533 1.8856 0.0072 0 0 0 0 0 1 9 1.4669 −0.5073 −0.0007−0.0261 0.0032 0 0 0 0 0 1 10 2.0773 −1.1689 −0.0485 −1.718 0.0095 0 0 00 0 1 11 −0.8957 −0.9498 −0.0091 −0.323 0.0031 0 0 0 0 0 1 12 −0.3021−1.806 0.0083 0.2942 0.0111 0 0 0 0 0 1 13 25.9974 0.7334 0.3505 12.40370.2894 0.1275 0 0 0 0 1 14 1.2968 0.9153 −0.0072 −0.2552 −0.0033 0 0 0 00 1 15 0.893 −1.0793 −0.0514 −1.8181 −0.0164 0 0 0 0 0 1 16 −3.6064−2.6611 −0.0589 −2.0841 −0.0103 0 0 0 0 0 2 1 36.4164 −9.1836 0.2247.9287 0.4854 0 0 0 0.25 0.1275 2 2 32.2119 −6.3228 0.3721 13.16840.4486 0 0 0 0.3571 0.1275 2 3 29.8229 −1.9943 0.4247 15.0311 0.3876 0 00 0.4643 0.1275 2 4 27.3051 1.7265 0.4455 15.7652 0.3255 0 0 0 0.57140.1275 2 5 22.2937 4.0704 0.4641 16.4261 0.2389 0 0 0 0.6786 0.1275 2 629.9281 2.3445 0.375 13.2711 0.3194 0 0 0 0.7857 0.1275 2 7 24.67971.8511 0.4513 15.9733 0.28 0 0 0 0.8929 0.1275 2 8 28.5064 −0.30510.3989 14.1171 0.2946 0 0 0 1 0.1275 2 9 38.4488 −15.6748 0.167 5.91040.5834 0 0 0 0 0.1275 2 10 40.0503 −15.804 0.1247 4.4135 0.5902 0 0 0 00.1275 2 11 33.9267 −10.9429 0.2674 9.463 0.5144 0 0 0 0 0.1275 2 1238.1132 −13.3928 0.2259 7.9943 0.5492 0 0 0 0 0.1275 2 13 34.3869−10.4026 0.257 9.0953 0.4914 0 0 0 0 0.1275 2 14 31.4203 −8.6136 0.27989.9036 0.4646 0 0 0 0 0.1275 2 15 29.7046 −7.6415 0.3448 12.2034 0.43010 0 0 0 0.1275 2 16 −1.8459 −1.4873 −0.0338 −1.1967 −0.0128 0 0 0 0 0 31 31.7288 −7.8872 0.2471 8.7457 0.4413 0 0 0 0.25 0.1275 3 2 34.0629−5.6821 0.256 9.0589 0.4354 0 0 0 0.3571 0.1275 3 3 29.4633 −2.79340.4371 15.4689 0.3748 0 0 0 0.4643 0.1275 3 4 30.2582 −0.7269 0.3813.4485 0.3535 0 0 0 0.5714 0.1275 3 5 29.4253 1.5896 0.3706 13.11410.3126 0 0 0 0.6786 0.1275 3 6 26.3528 1.2142 0.4479 15.8514 0.3145 0 00 0.7857 0.1275 3 7 25.601 3.7998 0.4435 15.696 0.2671 0 0 0 0.89290.1275 3 8 28.0192 0.1689 0.3905 13.8196 0.3192 0 0 0 1 0.1275 3 936.7685 −14.6028 0.1933 6.8418 0.585 0 0 0 0 0.1275 3 10 38.5741−13.8552 0.1662 5.8823 0.5767 0 0 0 0 0.1275 3 11 34.4052 −10.92050.2356 8.3394 0.5019 0 0 0 0 0.1275 3 12 35.2739 −11.206 0.2317 8.19870.5274 0 0 0 0 0.1275 3 13 33.0412 −8.7461 0.2758 9.7594 0.4592 0 0 0 00.1275 3 14 31.7936 −7.5655 0.2977 10.5345 0.423 0 0 0 0 0.1275 3 1529.6191 −5.2198 0.3214 11.374 0.3907 0 0 0 0 0.1275 3 16 3.3918 1.87260.022 0.777 −0.0062 0 0 0 0 0 4 1 30.7111 −6.7516 0.2778 9.8331 0.4345 00 0 0.25 0.1275 4 2 34.112 −8.2462 0.3332 11.7925 0.4978 0 0 0 0.35710.1275 4 3 33.5412 −4.8305 0.3278 11.5992 0.443 0 0 0 0.4643 0.1275 4 431.9087 −3.1967 0.3645 12.8999 0.3859 0 0 0 0.5714 0.1275 4 5 29.1731−1.3136 0.3976 14.0705 0.3672 0 0 0 0.6786 0.1275 4 6 28.959 1.89370.4366 15.4518 0.3113 0 0 0 0.7857 0.1275 4 7 26.9015 0.3211 0.399514.1375 0.3117 0 0 0 0.8929 0.1275 4 8 26.7599 −1.572 0.439 15.53640.3368 0 0 0 1 0.1275 4 9 36.6065 −14.1833 0.204 7.2199 0.5364 0 0 0 00.1275 4 10 37.5816 −14.2423 0.229 8.1061 0.5755 0 0 0 0 0.1275 4 1135.0624 −10.1028 0.2407 8.5191 0.5053 0 0 0 0 0.1275 4 12 33.2279−9.7613 0.2899 10.2593 0.4724 0 0 0 0 0.1275 4 13 34.1838 −7.8874 0.23248.2249 0.4515 0 0 0 0 0.1275 4 14 29.5376 −2.5807 0.2827 10.0032 0.37210 0 0 0 0.1275 4 15 30.3227 −4.5925 0.2567 9.083 0.4123 0 0 0 0 0.1275 416 22.7864 −1.4265 0.358 12.6711 0.3074 0.1275 0 0 0 0 5 1 30.9515−6.8352 0.2834 10.0285 0.4339 0 0 0 0.25 0.1275 5 2 33.089 −7.242 0.306910.8609 0.4608 0 0 0 0.3571 0.1275 5 3 30.0762 −2.4391 0.3773 13.35440.3784 0 0 0 0.4643 0.1275 5 4 29.2359 −1.2812 0.3524 12.4716 0.3598 0 00 0.5714 0.1275 5 5 27.9512 −0.1446 0.4363 15.4392 0.3348 0 0 0 0.67860.1275 5 6 27.6019 0.704 0.4437 15.7037 0.322 0 0 0 0.7857 0.1275 5 724.3249 2.9181 0.4752 16.8168 0.2789 0 0 0 0.8929 0.1275 5 8 26.76862.751 0.4201 14.8681 0.3014 0 0 0 1 0.1275 5 9 35.0835 −10.3253 0.2237.8906 0.5058 0 0 0 0 0.1275 5 10 34.9171 −11.3667 0.2561 9.0638 0.51140 0 0 0 0.1275 5 11 34.7082 −11.9114 0.2677 9.4727 0.498 0 0 0 0 0.12755 12 29.6627 −6.4427 0.3122 11.0487 0.406 0 0 0 0 0.1275 5 13 29.2257−5.8188 0.3176 11.2384 0.3854 0 0 0 0 0.1275 5 14 27.8848 −3.7179 0.327911.6036 0.3686 0 0 0 0 0.1275 5 15 26.1958 −2.7936 0.3298 11.6722 0.34330 0 0 0 0.1275 5 16 −0.1277 −1.924 −0.0092 −0.3246 0.0009 0 0 0 0 0 6 129.1389 −4.3012 0.3067 10.8556 0.3825 0 0 0 0.25 0.1275 6 2 31.6349−4.8533 0.3446 12.1966 0.4218 0 0 0 0.3571 0.1275 6 3 31.0745 −1.85260.3676 13.0108 0.3875 0 0 0 0.4643 0.1275 6 4 28.3213 −0.115 0.403914.2958 0.3501 0 0 0 0.5714 0.1275 6 5 26.3304 1.0766 0.4658 16.48640.3044 0 0 0 0.6786 0.1275 6 5 27.1453 1.0135 0.4055 14.3493 0.3351 0 00 0.7857 0.1275 6 7 26.8358 −0.3377 0.4188 14.8215 0.3128 0 0 0 0.89290.1275 6 8 25.1568 1.1966 0.4433 15.6885 0.3005 0 0 0 1 0.1275 6 932.6313 −9.608 0.2717 9.6147 0.4698 0 0 0 0 0.1275 6 10 33.6384 −8.64170.269 9.5214 0.4728 0 0 0 0 0.1275 6 11 33.7225 −9.2734 0.2814 9.95840.4685 0 0 0 0 0.1275 6 12 29.6467 −5.7142 0.3499 12.384 0.4007 0 0 0 00.1275 6 13 29.097 −3.77 0.3178 11.2482 0.3735 0 0 0 0 0.1275 6 1424.8397 −2.0416 0.3583 12.6797 0.3242 0 0 0 0 0.1275 6 15 23.8705 0.50420.3173 11.2304 0.2807 0 0 0 0 0.1275 6 16 −0.6023 −2.5656 −0.0204−0.7235 −0.0018 0 0 0 0 0 7 1 28.7119 −3.3592 0.2864 10.1361 0.3771 0 00 0.25 0.1275 7 2 29.2265 −1.4736 0.3597 12.7285 0.3607 0 0 0 0.35710.1275 7 3 27.4844 0.4723 0.4127 14.6073 0.3315 0 0 0 0.4643 0.1275 7 427.041 −0.0356 0.4391 15.5409 0.3275 0 0 0 0.5714 0.1275 7 5 27.16361.3548 0.4345 15.3776 0.3229 0 0 0 0.6786 0.1275 7 6 25.7661 1.93180.4599 16.2774 0.2965 0 0 0 0.7857 0.1275 7 7 23.3633 5.6157 0.458116.2107 0.2433 0 0 0 0.8929 0.1275 7 8 26.1496 1.1271 0.4805 17.00330.3089 0 0 0 1 0.1275 7 9 29.9105 −4.5145 0.3065 10.8484 0.3998 0 0 0 00.1275 7 10 29.2202 −4.8374 0.335 11.854 0.4013 0 0 0 0 0.1275 7 1128.1276 −3.2295 0.3683 13.035 0.3876 0 0 0 0 0.1275 7 12 24.7484 0.52550.3953 13.9896 0.3154 0 0 0 0 0.1275 7 13 21.1603 2.9377 0.3997 14.14570.2493 0 0 0 0 0.1275 7 14 20.7186 2.0292 0.4117 14.57 0.2644 0 0 0 00.1275 7 15 20.4604 3.3539 0.3891 13.7713 0.227 0 0 0 0 0.1275 7 16−0.528 0.6424 −0.0207 −0.7309 −0.0048 0 0 0 0 0 8 1 24.8909 0.06050.3107 10.9973 0.3123 0 0 0 0.25 0.1275 8 2 26.2546 1.6581 0.403 14.26320.322 0 0 0 0.3571 0.1275 8 3 27.1029 2.533 0.4101 14.5152 0.3139 0 0 00.4643 0.1275 8 4 24.6123 0.9852 0.4156 14.7095 0.3022 0 0 0 0.57140.1275 8 5 26.3109 2.7811 0.4426 15.6641 0.3122 0 0 0 0.6786 0.1275 8 623.0554 0.8878 0.441 15.6059 0.2956 0 0 0 0.7857 0.1275 8 7 24.39461.9018 0.4512 15.9688 0.2958 0 0 0 0.8929 0.1275 8 8 22.3853 4.13350.4599 16.2747 0.2618 0 0 0 1 0.1275 8 9 25.981 −3.4982 0.3065 10.84720.3615 0 0 0 0 0.1275 8 10 24.2313 0.0141 0.3603 12.7519 0.3139 0 0 0 00.1275 8 11 23.6274 −1.3834 0.3911 13.8418 0.3309 0 0 0 0 0.1275 8 1224.3757 1.2943 0.363 12.8451 0.2908 0 0 0 0 0.1275 8 13 20.9988 3.38770.3783 13.3874 0.2408 0 0 0 0 0.1275 8 14 20.0403 4.2559 0.3872 13.70370.2054 0 0 0 0 0.1275 8 15 17.311 2.637 0.3807 13.4747 0.2068 0 0 0 00.1275 8 16 0.5678 1.9726 −0.0464 −1.6434 −0.0159 0 0 0 0 0 9 1 30.9062−5.8046 0.2373 8.3989 0.4447 0 0.25 0 0 0.1275 9 2 31.6041 −5.58160.2994 10.5948 0.4491 0 0.375 0 0 0.1275 9 3 28.9111 −3.6802 0.301910.6838 0.4002 0 0.5 0 0 0.1275 9 4 26.2426 −4.1565 0.3558 12.5916 0.3880 0.625 0 0 0.1275 9 5 25.9149 −2.0835 0.3543 12.538 0.3543 0 0.75 0 00.1275 9 6 23.3901 2.4799 0.4266 15.0973 0.2851 0 0.875 0 0 0.1275 9 723.5644 0.8315 0.4172 14.7632 0.3115 0 1 0 0 0.1275 9 8 26.6687 1.03060.384 13.5909 0.3579 0.1275 0 0 0 0 9 9 20.9817 0.7358 0.4114 14.55910.2682 0 0 0 0 0.1275 9 10 20.2046 4.3735 0.3698 13.0857 0.2173 0 0 0 00.1275 9 11 20.0105 4.013 0.41 14.5099 0.2217 0 0 0 0 0.1275 9 1219.4493 5.5974 0.4104 14.5225 0.1907 0 0 0 0 0.1275 9 13 16.9213 5.50290.4634 16.4005 0.1918 0 0 0 0 0.1275 9 14 16.1597 7.4264 0.4133 14.62590.1599 0 0 0 0 0.1275 9 15 15.3887 6.9817 0.4329 15.3209 0.1508 0 0 0 00.1275 9 16 1.48 1.6733 0.042 1.4871 0.0069 0 0 0 3 0 10 1 30.6968−10.2541 0.2847 10.0774 0.476 0 0.25 0 0 0.1275 10 2 32.1255 −11.07420.2959 10.4703 0.514 0 0.375 0 0 0.1275 10 3 32.1474 −9.1654 0.300510.6363 0.4622 0 0.5 0 0 0.1275 10 4 30.6915 −6.0781 0.3187 11.27850.4306 0 0.625 0 0 0.1275 10 5 27.9014 −2.5207 0.3728 13.195 0.3638 00.75 0 0 0.1275 10 6 26.7893 0.1041 0.3791 13.4175 0.3212 0 0.875 0 00.1275 10 7 25.6916 −1.6411 0.4001 14.1593 0.3168 0 1 0 0 0.1275 10 840.7148 −14.9327 0.1956 6.9208 0.6111 0 0 0.25 0 0.1275 10 9 37.6203−11.5739 0.2772 9.8117 0.5535 0 0 0.3571 0 0.1275 10 10 36.0618 −9.65520.2772 9.8098 0.5182 0 0 0.4643 0 0.1275 10 11 33.6683 −7.9074 0.335211.8612 0.4994 0 0 0.5714 0 0.1275 10 12 30.8619 −2.9942 0.383 13.55480.4254 0 0 0.6786 0 0.1275 10 13 27.3645 −0.1824 0.4576 16.1951 0.3507 00 0.7857 0 0.1275 10 14 25.9153 0.8696 0.4335 15.3422 0.3058 0 0 0.89290 0.1275 10 15 24.8832 2.3622 0.381 13.4835 0.2884 0 0 1 0 0.1275 10 1622.1513 −0.11 0.3618 12.8028 0.3028 0.1275 0 0 0 0 11 1 29.6722 −10.17130.296 10.4745 0.4751 0 0.25 0 0 0.1275 11 2 31.7003 −8.8368 0.297110.5137 0.4694 0 0.375 0 0 0.1275 11 3 29.2951 −7.329 0.318 11.25360.4393 0 0.5 0 0 0.1275 11 4 28.0821 −5.9298 0.3618 12.8032 0.4019 00.625 0 0 0.1275 11 5 24.5742 −1.3821 0.3883 13.7409 0.3116 0 0.75 0 00.1275 11 5 24.4104 2.6657 0.3931 13.9121 0.2679 0 0.875 0 0 0.1275 11 723.7364 0.5167 0.414 14.6505 0.2856 0 1 0 0 0.1275 11 8 38.1522 −11.4360.2798 9.9026 0.5515 0 0 0.25 0 0.1275 11 9 35.6744 −12.1263 0.331911.7465 0.5375 0 0 0.3571 0 0.1275 11 10 33.8417 −8.2101 0.3352 11.86370.4848 0 0 0.4643 0 0.1275 11 11 32.3206 −5.8536 0.3718 13.1565 0.4522 00 0.5714 0 0.1275 11 12 29.8353 −3.4642 0.4367 15.4552 0.379 0 0 0.67860 0.1275 11 13 24.3129 0.2244 0.4599 16.2759 0.3141 0 0 0.7857 0 0.127511 14 23.9117 0.8021 0.4431 15.6801 0.2893 0 0 0.8929 0 0.1275 11 1522.5909 2.0424 0.4437 15.7032 0.2739 0 0 1 0 0.1275 11 16 −0.1216 0.5666−0.0089 −0.3161 0.001 0 0 0 0 0 12 1 29.8448 −9.8277 0.3071 10.86850.461 0 0.25 0 0 0.1275 12 2 31.3438 −8.3043 0.3182 11.2609 0.4598 00.375 0 0 0.1275 12 3 30.9513 −7.388 0.3256 11.5218 0.456 0 0.5 0 00.1275 12 4 26.2462 −2.6572 0.4142 14.658 0.3618 0 0.625 0 0 0.1275 12 522.892 0.8639 0.4339 15.3574 0.2889 0 0.75 0 0 0.1275 12 6 21.62193.8697 0.4452 15.7571 0.2409 0 0.875 0 0 0.1275 12 7 19.9189 4.93130.4639 16.4169 0.2165 0 1 0 0 0.1275 12 8 34.5283 −10.7244 0.335411.8715 0.5122 0 0 0.25 0 0.1275 12 9 33.9857 −8.2047 0.343 12.13840.4815 0 0 0.3571 0 0.1275 12 10 31.621 −4.3118 0.3546 12.5489 0.4314 00 0.4643 0 0.1275 12 11 29.2723 −5.1635 0.4313 15.2636 0.4023 0 0 0.57140 0.1275 12 12 27.2007 −1.0088 0.4189 14.8237 0.3493 0 0 0.6786 0 0.127512 13 23.1362 0.634 0.4647 16.4447 0.2984 0 0 0.7857 0 0.1275 12 1423.2574 2.1268 0.4286 15.1689 0.2725 0 0 0.8929 0 0.1275 12 15 21.24691.8488 0.4443 15.7235 0.2656 0 0 1 0 0.1275 12 16 −1.1045 −0.8366−0.0103 −0.3662 0.0014 0 0 0 0 0 13 1 25.7035 −7.1229 0.3295 11.66230.3923 0 0.25 0 0 0.1275 13 2 27.9296 −4.9293 0.3516 12.4415 0.3851 00.375 0 0 0.1275 13 3 26.5836 −2.6903 0.3387 11.9859 0.3703 0 0.5 0 00.1275 13 4 25.0695 −2.3513 0.3803 13.4579 0.3398 0 0.625 0 0 0.1275 135 24.2518 −2.8024 0.3952 13.9866 0.3243 0 0.75 0 0 0.1275 13 6 19.07862.9081 0.4389 15.5314 0.2246 0 0.875 0 0 0.1275 13 7 18.2324 6.92460.4827 17.0843 0.1918 0 1 0 0 0.1275 13 8 30.5494 −2.9391 0.3997 14.14580.4164 0 0 0.25 0 0.1275 13 9 30.9918 −5.3314 0.3674 13.0007 0.4358 0 00.3571 0 0.1275 13 10 26.763 −0.2578 0.4077 14.4275 0.3345 0 0 0.4643 00.1275 13 11 23.8381 0.2053 0.4628 16.3779 0.3142 0 0 0.5714 0 0.1275 1312 24.4559 1.1055 0.4518 15.9889 0.3077 0 0 0.6786 0 0.1275 13 1322.6291 3.7132 0.4594 16.2587 0.2702 0 0 0.7857 0 0.1275 13 14 22.0582.8756 0.4643 16.4327 0.2575 0 0 0.8929 0 0.1275 13 15 21.6325 4.21590.4687 16.5861 0.2498 0 0 1 0 0.1275 13 16 −1.6445 0.0792 0.0082 0.29130.0011 0 0 0 0 0 14 1 23.1422 −2.3558 0.3575 12.6536 0.334 0 0.25 0 00.1275 14 2 23.5238 −0.901 0.3988 14.1123 0.3236 0 0.375 0 0 0.1275 14 322.0837 0.8748 0.406 14.3686 0.2887 0 0.5 0 0 0.1275 14 4 22.8759 2.55740.3834 13.5696 0.2754 0 0.625 0 0 0.1275 14 5 19.1287 4.7184 0.43315.3226 0.2341 0 0.75 0 0 0.1275 14 6 16.1516 6.2373 0.4614 16.33050.1783 0 0.875 0 0 0.1275 14 7 15.767 8.7722 0.4915 17.3958 0.1456 0 1 00 0.1275 14 8 26.1629 0.3617 0.428 15.1475 0.3377 0 0 0.25 0 0.1275 14 927.6928 −0.3316 0.3895 13.7834 0.3418 0 0 0.3571 0 0.1275 14 10 23.63232.0136 0.4199 14.8589 0.2944 0 0 0.4643 0 0.1275 14 11 22.9238 3.49490.4318 15.2811 0.2599 0 0 0.5714 0 0.1275 14 12 20.0974 3.9245 0.461516.331 0.2382 0 0 0.6786 0 0.1275 14 13 20.8567 4.1929 0.4532 16.03990.2401 0 0 0.7857 0 0.1275 14 14 20.5092 3.8209 0.4542 16.0726 0.246 0 00.8929 0 0.1275 14 15 19.5783 3.9669 0.4226 14.9574 0.2347 0 0 1 00.1275 14 16 −1.2663 0.2287 0.0049 0.1744 0.0028 0 0 0 0 0 15 1 19.71751.5028 0.4362 15.4385 0.251 0 0.25 0 0 0.1275 15 2 18.0113 3.3898 0.370513.1108 0.2201 0 0.375 0 0 0.1275 15 3 15.9884 3.6197 0.375 13.27110.2024 0 0.5 0 0 0.1275 15 4 14.8384 6.1755 0.3784 13.3915 0.1718 00.625 0 0 0.1275 15 5 17.968 4.6171 0.3723 13.1769 0.2031 0 0.75 0 00.1275 15 6 12.6392 8.1823 0.4391 15.54 0.1278 0 0.875 0 0 0.1275 15 712.908 10.31 0.421 14.899 0.1178 0 1 0 0 0.1275 15 8 22.4908 3.75630.4451 15.7514 0.2796 0 0 0.25 0 0.1275 15 9 20.5065 4.7112 0.426515.0938 0.2479 0 0 0.3571 0 0.1275 15 10 20.472 5.2749 0.4461 15.78590.2487 0 0 0.4643 0 0.1275 15 11 19.2131 5.2423 0.4553 16.1141 0.2276 00 0.5714 0 0.1275 15 12 19.315 5.6034 0.4378 15.4948 0.222 0 0 0.6786 00.1275 15 13 19.2915 5.4631 0.4068 14.3951 0.2215 0 0 0.7857 0 0.1275 1514 19.5125 4.9808 0.4193 14.8397 0.2264 0 0 0.8929 0 0.1275 15 1519.5687 5.6104 0.4234 14.9856 0.2286 0 0 1 0 0.1275 15 16 1.5744 2.08660.0612 2.1664 0.0059 0 0 0 0 0 16 1 15.3115 8.3071 0.4772 16.8896 0.13890 0.25 0 0 0.1275 16 2 5.2619 4.7062 0.2088 7.3912 0.0611 0 0.375 0 00.1275 16 3 4.8009 4.1018 0.1945 6.8835 0.0422 0 0.5 0 0 0.1275 16 43.6868 3.1471 0.1868 6.6103 0.0426 0 0.625 0 0 0.1275 16 5 6.4671 6.21390.2776 9.8227 0.0482 0 0.75 0 0 0.1275 16 6 10.0153 8.3873 0.388913.7622 0.0946 0 0.875 0 0 0.1275 16 7 9.1584 7.6145 0.405 14.33260.0867 0 1 0 0 0.1275 16 8 20.3819 3.6436 0.397 14.051 0.2505 0 0 0.25 00.1275 16 9 20.4977 2.9382 0.3951 13.9812 0.2412 0 0 0.3571 0 0.1275 1610 17.6443 2.4709 0.3937 13.9331 0.2379 0 0 0.4643 0 0.1275 16 1117.6931 2.9484 0.3976 14.0709 0.2315 0 0 0.5714 0 0.1275 16 12 14.46591.353 0.3206 11.3452 0.2104 0 0 0.6786 0 0.1275 16 13 14.2303 1.27460.2638 9.3376 0.1943 0 0 0.7857 0 0.1275 16 14 14.9027 1.4698 0.327311.5832 0.2194 0 0 0.8929 0 0.1275 16 15 12.5533 1.487 0.2375 8.4060.1927 0 0 1 0 0.1275 16 16 20.3125 2.973 0.4288 15.1746 0.2463 0.1275 00 0 0 Tem- pera- ture: 350 C. SUM_(—) mol % mol % mol % mol % mol % mol% R C RuNONO33 ZrONO32 micromols Fe La Ti Pt Ru Zr real real real real 11 0 0 0.1275 0 0 0 100 0 0 1 2 0 0 0 0 0 0 0 0 0 1 3 0 0 0 0 0 0 0 0 0 14 0 0 0 0 0 0 0 0 0 1 5 0 0 0 0 0 0 0 0 0 1 6 0 0 0 0 0 0 0 0 0 1 7 0 00.1275 0 0 0 100 0 0 1 8 0 0 0 0 0 0 0 0 0 1 9 0 0 0 0 0 0 0 0 0 1 10 00 0 0 0 0 0 0 0 1 11 0 0 0 0 0 0 0 0 0 1 12 0 0 0 0 0 0 0 0 0 1 13 0 00.1275 0 0 0 100 0 0 1 14 0 0 0 0 0 0 0 0 0 1 15 0 0 0 0 0 0 0 0 0 1 160 0 0 0 0 0 0 0 0 2 1 0.0989 0 0.4764 0 0 52.48 26.76 20.76 0 2 2 0.09890 0.5835 0 0 61.2 21.85 16.95 0 2 3 0.0989 0 0.6907 0 0 67.22 18.4614.32 0 2 4 0.0989 0 0.7978 0 0 71.62 15.98 12.4 0 2 5 0.0989 0 0.905 00 74.98 14.09 10.93 0 2 6 0.0989 0 1.0121 0 0 77.63 12.6 9.77 0 2 70.0989 0 1.1193 0 0 79.77 11.39 8.84 0 2 8 0.0989 0 1.2264 0 0 81.5410.4 8.06 0 2 9 0.0989 0.25 0.4764 0 0 0 26.76 20.76 52.48 2 10 0.09890.375 0.6014 0 0 0 21.2 16.44 62.35 2 11 0.0989 0.5 0.7264 0 0 0 17.5513.62 68.83 2 12 0.0989 0.625 0.8514 0 0 0 14.98 11.62 73.41 2 13 0.09890.75 0.9764 0 0 0 13.06 10.13 76.81 2 14 0.0989 0.875 1.1014 0 0 0 11.588.98 79.44 2 15 0.0989 1 1.2264 0 0 0 10.4 8.06 81.54 2 16 0 0 0 0 0 0 00 0 3 1 0.0865 0 0.464 0 0 53.87 27.48 18.65 0 3 2 0.0865 0 0.5712 0 062.53 22.32 15.15 0 3 3 0.0865 0 0.6783 0 0 68.45 18.8 12.76 0 3 40.0865 0 0.7855 0 0 72.75 16.23 11.02 0 3 5 0.0865 0 0.8926 0 0 76.0214.28 9.69 0 3 6 0.0865 0 0.9998 0 0 78.59 12.75 8.66 0 3 7 0.0865 01.1069 0 0 80.66 11.52 7.82 0 3 8 0.0865 0 1.214 0 0 82.37 10.5 7.13 0 39 0.0883 0.25 0.4658 0 0 0 27.37 18.96 53.67 3 10 0.0883 0.375 0.5908 00 0 21.58 14.95 63.47 3 11 0.0883 0.5 0.7158 0 0 0 17.81 12.34 69.85 312 0.0883 0.625 0.8408 0 0 0 15.16 10.5 74.33 3 13 0.0883 0.75 0.9658 00 0 13.2 9.14 77.66 3 14 0.0883 0.875 1.0908 0 0 0 11.69 8.1 80.22 3 150.0883 1 1.2158 0 0 0 10.49 7.26 82.25 3 16 0 0 0 0 0 0 0 0 0 4 1 0.07420 0.4517 0 0 55.35 28.23 16.42 0 4 2 0.0742 0 0.5588 0 0 63.91 22.8213.27 0 4 3 0.0742 0 0.666 0 0 69.72 19.15 11.14 0 4 4 0.0742 0 0.7731 00 73.91 16.49 9.59 0 4 5 0.0742 0 0.8802 0 0 77.09 14.48 8.43 0 4 60.0742 0 0.9874 0 0 79.57 12.91 7.51 0 4 7 0.0742 0 1.0945 0 0 81.5711.65 6.78 0 4 8 0.0742 0 1.2017 0 0 83.22 10.61 6.17 0 4 9 0.0777 0.250.4552 0 0 0 28.01 17.07 54.92 4 10 0.0777 0.375 0.5802 0 0 0 21.9713.39 64.63 4 11 0.0777 0.5 0.7052 0 0 0 18.08 11.02 70.9 4 12 0.07770.625 0.8302 0 0 0 15.36 9.36 75.28 4 13 0.0777 0.75 0.9552 0 0 0 13.358.14 78.52 4 14 0.0777 0.875 1.0802 0 0 0 11.8 7.19 81 4 15 0.0777 11.2052 0 0 0 10.58 6.45 82.97 4 16 0 0 0.1275 0 0 0 100 0 0 5 1 0.0618 00.4393 0 0 56.91 29.02 14.07 0 5 2 0.0618 0 0.5465 0 0 65.36 23.33 11.310 5 3 0.0618 0 0.6536 0 0 71.04 19.51 9.46 0 5 4 0.0618 0 0.7607 0 075.11 16.76 8.13 0 5 5 0.0618 0 0.8679 0 0 78.19 14.69 7.12 0 5 6 0.06180 0.975 0 0 80.58 13.08 6.34 0 5 7 0.0618 0 1.0822 0 0 82.51 11.78 5.710 5 8 0.0618 0 1.1893 0 0 84.08 10.72 5.2 0 5 9 0.0671 0.25 0.4446 0 0 028.68 15.09 56.23 5 10 0.0671 0.375 0.5696 0 0 0 22.38 11.78 65.83 5 110.0671 0.5 0.6946 0 0 0 18.36 9.66 71.98 5 12 0.0671 0.625 0.8196 0 0 015.56 8.19 76.26 5 13 0.0671 0.75 0.9446 0 0 0 13.5 7.1 79.4 5 14 0.06710.875 1.0696 0 0 0 11.92 6.27 81.81 5 15 0.0671 1 1.1946 0 0 0 10.675.62 83.71 5 16 0 0 0 0 0 0 0 0 0 6 1 0.0495 0 0.427 0 0 58.5529.86298161 11.58215248 0 6 2 0.0495 0 0.5341 0 0 66.87 23.87 9.26 0 6 30.0495 0 0.6412 0 0 72.4 19.88 7.71 0 6 4 0.0495 0 0.7484 0 0 76.3617.04 6.61 0 6 5 0.0495 0 0.8555 0 0 79.32 14.9 5.78 0 6 5 0.0495 00.9627 0 0 81.62 13.24 5.14 0 6 7 0.0495 0 1.0698 0 0 83.46 11.92 4.62 06 8 0.0495 0 1.177 0 0 84.97 10.83 4.2 0 6 9 0.0565 0.25 0.434 0 0 029.38 13.02 57.6 6 10 0.0565 0.375 0.559 0 0 0 22.81 10.11 67.08 6 110.0565 0.5 0.684 0 0 0 18.64 8.26 73.1 6 12 0.0565 0.625 0.809 0 0 015.76 6.99 77.25 6 13 0.0565 0.75 0.934 0 0 0 13.65 6.05 80.3 6 140.0565 0.875 1.059 0 0 0 12.04 5.34 82.62 6 15 0.0565 1 1.184 0 0 010.77 4.77 84.46 6 16 0 0 0 0 0 0 0 0 0 7 1 0.0371 0 0.4146 0 0 60.330.75 8.95 0 7 2 0.0371 0 0.5217 0 0 68.45 24.44 7.11 0 7 3 0.0371 00.6289 0 0 73.83 20.27 5.9 0 7 4 0.0371 0 0.736 0 0 77.64 17.32 5.04 0 75 0.0371 0 0.8432 0 0 80.48 15.12 4.4 0 7 6 0.0371 0 0.9503 0 0 82.6813.42 3.9 0 7 7 0.0371 0 1.0574 0 0 84.44 12.06 3.51 0 7 8 0.0371 01.1646 0 0 85.87 10.95 3.18 0 7 9 0.0459 0.25 0.4234 0 0 0 30.11 10.8459.04 7 10 0.0459 0.375 0.5484 0 0 0 23.25 8.37 68.38 7 11 0.0459 0.50.6734 0 0 0 18.93 6.82 74.25 7 12 0.0459 0.625 0.7984 0 0 0 15.97 5.7578.28 7 13 0.0459 0.75 0.9234 0 0 0 13.81 4.97 81.22 7 14 0.0459 0.8751.0484 0 0 0 12.16 4.38 83.46 7 15 0.0459 1 1.1734 0 0 0 10.87 3.9185.22 7 16 0 0 0 0 0 0 0 0 0 8 1 0.0247 0 0.4022 0 0 62.15 31.7 6.15 0 82 0.0247 0 0.5094 0 0 70.11 25.03 4.85 0 8 3 0.0247 0 0.6165 0 0 75.3120.68 4.01 0 8 4 0.0247 0 0.7237 0 0 78.96 17.62 3.42 0 8 5 0.0247 00.8308 0 0 81.68 15.35 2.98 0 8 6 0.0247 0 0.9379 0 0 83.77 13.59 2.64 08 7 0.0247 0 1.0451 0 0 85.43 12.2 2.37 0 8 8 0.0247 0 1.1522 0 0 86.7911.07 2.15 0 8 9 0.0353 0.25 0.4128 0 0 0 30.89 8.56 60.56 8 10 0.03530.375 0.5378 0 0 0 23.71 6.57 69.73 8 11 0.0353 0.5 0.6628 0 0 0 19.245.33 75.44 8 12 0.0353 0.625 0.7878 0 0 0 16.18 4.48 79.33 8 13 0.03530.75 0.9128 0 0 0 13.97 3.87 82.16 8 14 0.0353 0.875 1.0378 0 0 0 12.293.4 84.31 8 15 0.0353 1 1.1628 0 0 0 10.96 3.04 86 8 16 0 0 0 0 0 0 0 00 9 1 0.0989 0 0.4764 52.48 0 0 26.76 20.76 0 9 2 0.0989 0 0.6014 62.350 0 21.2 16.44 0 9 3 0.0989 0 0.7264 68.83 0 0 17.55 13.62 0 9 4 0.09890 0.8514 73.41 0 0 14.98 11.62 0 9 5 0.0989 0 0.9764 76.81 0 0 13.0610.13 0 9 6 0.0989 0 1.1014 79.44 0 0 11.58 8.98 0 9 7 0.0989 0 1.226481.54 0 0 10.4 8.06 0 9 8 0 0 0.1275 0 0 0 100 0 0 9 9 0.0247 0.250.4022 0 0 0 31.7 6.15 62.15 9 10 0.0247 0.375 0.5272 0 0 0 24.18 4.6971.13 9 11 0.0247 0.5 0.6522 0 0 0 19.55 3.79 76.66 9 12 0.0247 0.6250.7772 0 0 0 16.4 3.18 80.41 9 13 0.0247 0.75 0.9022 0 0 0 14.13 2.7483.13 9 14 0.0247 0.875 1.0272 0 0 0 12.41 2.41 85.18 9 15 0.0247 11.1522 0 0 0 11.07 2.15 86.79 9 16 0 0 0 0 0 0 0 0 0 10 1 0.0883 00.4658 53.67 0 0 27.37 18.96 0 10 2 0.0883 0 0.5908 63.47 0 0 21.5814.95 0 10 3 0.0883 0 0.7158 69.85 0 0 17.81 12.34 0 10 4 0.0883 00.8408 74.33 0 0 15.16 10.5 0 10 5 0.0883 0 0.9658 77.66 0 0 13.2 9.14 010 6 0.0883 0 1.0908 80.22 0 0 11.69 8.1 0 10 7 0.0883 0 1.2158 82.25 00 10.49 7.26 0 10 8 0.0989 0 0.4764 0 52.48 0 26.76 20.76 0 10 9 0.09890 0.5835 0 61.2 0 21.85 16.95 0 10 10 0.0989 0 0.6907 0 67.22 0 18.4614.32 0 10 11 0.0989 0 0.7978 0 71.62 0 15.98 12.4 0 10 12 0.0989 00.905 0 74.98 0 14.09 10.93 0 10 13 0.0989 0 1.0121 0 77.63 0 12.6 9.770 10 14 0.0989 0 1.1193 0 79.77 0 11.39 8.84 0 10 15 0.0989 0 1.2264 081.54 0 10.4 8.06 0 10 16 0 0 0.1275 0 0 0 100 0 0 11 1 0.0777 0 0.455254.92 0 0 28.01 17.07 0 11 2 0.0777 0 0.5802 64.63 0 0 21.97 13.39 0 113 0.0777 0 0.7052 70.9 0 0 18.08 11.02 0 11 4 0.0777 0 0.8302 75.28 0 015.36 9.36 0 11 5 0.0777 0 0.9552 78.52 0 0 13.35 8.14 0 11 5 0.0777 01.0802 81 0 0 11.8 7.19 0 11 7 0.0777 0 1.2052 82.97 0 0 10.58 6.45 0 118 0.0865 0 0.464 0 53.87 0 27.48 18.65 0 11 9 0.0865 0 0.5712 0 62.53 022.32 15.15 0 11 10 0.0865 0 0.6783 0 68.45 0 18.8 12.76 0 11 11 0.08650 0.7855 0 72.75 0 16.23 11.02 0 11 12 0.0865 0 0.8926 0 76.02 0 14.289.69 0 11 13 0.0865 0 0.9998 0 78.59 0 12.75 8.66 0 11 14 0.0865 01.1069 0 80.66 0 11.52 7.82 0 11 15 0.0865 0 1.214 0 82.37 0 10.5 7.13 011 16 0 0 0 0 0 0 0 0 0 12 1 0.0671 0 0.4446 56.23 0 0 28.68 15.09 0 122 0.0671 0 0.5696 65.83 0 0 22.38 11.78 0 12 3 0.0671 0 0.6946 71.98 0 018.36 9.66 0 12 4 0.0671 0 0.8196 76.26 0 0 15.56 8.19 0 12 5 0.0671 00.9446 79.4 0 0 13.5 7.1 0 12 6 0.0671 0 1.0696 81.81 0 0 11.92 6.27 012 7 0.0671 0 1.1946 83.71 0 0 10.67 5.62 0 12 8 0.0742 0 0.4517 0 55.350 28.23 16.42 0 12 9 0.0742 0 0.5588 0 63.91 0 22.82 13.27 0 12 100.0742 0 0.666 0 69.72 0 19.15 11.14 0 12 11 0.0742 0 0.7731 0 73.91 016.49 9.59 0 12 12 0.0742 0 0.8802 0 77.09 0 14.48 8.43 0 12 13 0.0742 00.9874 0 79.57 0 12.91 7.51 0 12 14 0.0742 0 1.0945 0 81.57 0 11.65 6.780 12 15 0.0742 0 1.2017 0 83.22 0 10.61 6.17 0 12 16 0 0 0 0 0 0 0 0 013 1 0.0565 0 0.434 57.6 0 0 29.37691318 13.02129626 0 13 2 0.0565 00.559 67.08 0 0 22.80800387 10.1096318 0 13 3 0.0565 0 0.684 73.1 0 018.63996156 8.262149952 0 13 4 0.0565 0 0.809 77.25 0 0 15.759919476.985573305 0 13 5 0.0565 0 0.934 80.3 0 0 13.6507548 6.050687537 0 13 60.0565 0 1.059 82.62 0 0 12.03949764 5.336498926 0 13 7 0.0565 0 1.18484.46 0 0 10.76845115 4.773108456 0 13 8 0.0618 0 0.4393 0 56.91 029.02262057 14.07028027 0 13 9 0.0618 0 0.5465 0 65.36 0 23.3321890511.31153675 0 13 10 0.0618 0 0.6536 0 71.04 0 19.50739766 9.457262887 013 11 0.0618 0 0.7607 0 75.11 0 16.75997261 8.125300447 0 13 12 0.0618 00.8679 0 78.19 0 14.69090509 7.122208397 0 13 13 0.0618 0 0.975 0 80.580 13.07656404 6.339569528 0 13 14 0.0618 0 1.0822 0 82.51 0 11.781886735.711904889 0 13 15 0.0618 0 1.1893 0 84.08 0 10.72047927 5.19733039 013 16 0 0 0 0 0 0 0 0 0 14 1 0.0459 0 0.4234 59.04 0 0 30.11 10.84 0 142 0.0459 0 0.5484 68.38 0 0 23.25 8.37 0 14 3 0.0459 0 0.6734 74.25 0 018.93 6.82 0 14 4 0.0459 0 0.7984 78.28 0 0 15.97 5.75 0 14 5 0.0459 00.9234 81.22 0 0 13.81 4.97 0 14 6 0.0459 0 1.0484 83.46 0 0 12.16 4.380 14 7 0.0459 0 1.1734 85.22 0 0 10.87 3.91 0 14 8 0.0495 0 0.427 058.55 0 29.86 11.58 0 14 9 0.0495 0 0.5341 0 66.87 0 23.87 9.26 0 14 100.0495 0 0.6412 0 72.4 0 19.88 7.71 0 14 11 0.0495 0 0.7484 0 76.36 017.04 6.61 0 14 12 0.0495 0 0.8555 0 79.32 0 14.9 5.78 0 14 13 0.0495 00.9627 0 81.62 0 13.24 5.14 0 14 14 0.0495 0 1.0698 0 83.46 0 11.92 4.620 14 15 0.0495 0 1.177 0 84.97 0 10.83 4.2 0 14 16 0 0 0 0 0 0 0 0 0 151 0.0353 0 0.4128 60.56 0 0 30.89 8.56 0 15 2 0.0353 0 0.5378 69.73 0 023.71 6.57 0 15 3 0.0353 0 0.6628 75.44 0 0 19.24 5.33 0 15 4 0.0353 00.7878 79.33 0 0 16.18 4.48 0 15 5 0.0353 0 0.9128 82.16 0 0 13.97 3.870 15 6 0.0353 0 1.0378 84.31 0 0 12.29 3.4 0 15 7 0.0353 0 1.1628 86 0 010.96 3.04 0 15 8 0.0371 0 0.4146 0 60.3 0 30.75 8.95 0 15 9 0.0371 00.5217 0 68.45 0 24.44 7.11 0 15 10 0.0371 0 0.6289 0 73.83 0 20.27 5.90 15 11 0.0371 0 0.736 0 77.64 0 17.32 5.04 0 15 12 0.0371 0 0.8432 080.48 0 15.12 4.4 0 15 13 0.0371 0 0.9503 0 82.68 0 13.42 3.9 0 15 140.0371 0 1.0574 0 84.44 0 12.06 3.51 0 15 15 0.0371 0 1.1646 0 85.87 010.95 3.18 0 15 16 0 0 0 0 0 0 0 0 0 16 1 0.0247 0 0.4022 62.15 0 0 31.76.15 0 16 2 0.0247 0 0.5272 71.13 0 0 24.18 4.69 0 16 3 0.0247 0 0.652276.66 0 0 19.55 3.79 0 16 4 0.0247 0 0.7772 80.41 0 0 16.4 3.18 0 16 50.0247 0 0.9022 83.13 0 0 14.13 2.74 0 16 6 0.0247 0 1.0272 85.18 0 012.41 2.41 0 16 7 0.0247 0 1.1522 86.79 0 0 11.07 2.15 0 16 8 0.0247 00.4022 0 62.15 0 31.7 6.15 0 16 9 0.0247 0 0.5094 0 70.11 0 25.03 4.85 016 10 0.0247 0 0.6165 0 75.31 0 20.68 4.01 0 16 11 0.0247 0 0.7237 078.96 0 17.62 3.42 0 16 12 0.0247 0 0.8308 0 81.68 0 15.35 2.98 0 16 130.0247 0 0.9379 0 83.77 0 13.59 2.64 0 16 14 0.0247 0 1.0451 0 85.43 012.2 2.37 0 16 15 0.0247 0 1.1522 0 86.79 0 11.07 2.15 0 16 16 0 00.1275 0 0 0 100 0 0

[0298] Table IV Tem- pera- ture: 300 C. Pt1.0%/ R C COCONV H2OCONVCO2PROD CO2PERPROD CH4PROD ZrO2std CoNO32 FeNO33 GeOX2 H2MoO4 LaNO33real real real real real real real real real real real real real 1 125.8564 17.3624 0.9641 34.8524 0.1872 0.1275 0 0 0 0 0 1 2 −3.5288−1.0034 0.0465 1.6792 0.0188 0 0 0 0 0 0 1 3 −3.2594 −1.1661 0.01660.5998 0.0121 0 0 0 0 0 0 1 4 −2.9732 −3.7232 0.008 0.2881 0.0087 0 0 00 0 0 1 5 −2.8279 −4.1686 −0.0176 −0.636 0.0037 0 0 0 0 0 0 1 6 −0.8995−1.8273 0.0207 0.7469 0.007 0 0 0 0 0 0 1 7 29.8929 15.3753 0.947534.2529 0.1713 0.1275 0 0 0 0 0 1 8 0.2455 −0.7786 0.0364 1.317 0.0059 00 0 0 0 0 1 9 1.8628 1.8933 0.0797 2.8821 0.0104 0 0 0 0 0 0 1 10−1.0457 −1.7441 −0.0214 −0.7745 0.0034 0 0 0 0 0 0 1 11 −0.9415 −1.632−0.0272 −0.9819 −0.0032 0 0 0 0 0 0 1 12 −1.4473 −2.099 −0.0436 −1.5778−0.0067 0 0 0 0 0 0 1 13 29.7322 15.3824 0.922 33.3294 0.1512 0.1275 0 00 0 0 1 14 −0.4246 −0.0063 −0.0224 −0.8114 −0.005 0 0 0 0 0 0 1 15−0.9697 −0.7029 −0.0374 −1.3523 −0.0056 0 0 0 0 0 0 1 16 32.2511 15.09750.9551 34.5247 0.1837 0.1275 0 0 0 0 0 2 1 25.7402 15.132 0.821 29.67790.1024 0 0 1 0 0 0 2 2 23.6205 13.0894 0.7368 26.6334 0.0932 0 0 1 0 0 02 3 22.2339 13.8399 0.7116 25.7223 0.0904 0 0 1 0 0 0 2 4 10.2788 6.05040.3053 11.0365 0.0334 0 0 1 0 1 0 2 5 24.8097 18.3968 0.7586 27.42460.0984 0 1 1 0 0 0 2 6 30.7805 17.4659 0.9424 34.0689 0.1445 0 0 0 0 0 02 7 24.5818 17.5787 0.7641 27.6231 0.1029 0 0 0 0 0 0 2 8 30.048318.2382 1.0024 36.2373 0.1267 0 0 0 0 0 0 2 9 8.9325 5.5702 0.275 9.93970.0302 0 0 0 0 1 0 2 10 48.0297 −3.6479 0.6535 23.6248 0.5638 0 1 0 0 00 2 11 33.7357 12.0981 0.8374 30.2711 0.2395 0 0 0 0 0 0 2 12 25.018512.5103 0.7266 26.268 0.133 0 0 0 0 0 0 2 13 32.2828 17.7494 1.015736.7159 0.148 0 0 0 0 0 0 2 14 14.7003 10.1762 0.4613 16.6741 0.0611 0 00 0 1 0 2 15 40.8678 6.002 0.8233 29.7614 0.3924 0 1 0 0 0 0 2 16−0.6906 −1.1865 −0.0214 −0.7728 −0.0011 0 0 0 0 0 0 3 1 25.0677 15.22870.7962 28.781 0.0976 0 0 0.875 0 0 0 3 2 21.7886 14.5137 0.6935 25.07150.0867 0 0 0.875 0 0 0 3 3 23.5288 15.7457 0.7124 25.7537 0.0872 0 00.875 0 0 0 3 4 10.7835 7.3033 0.3034 10.9679 0.0327 0 0 0.875 0 0.875 03 5 35.9677 7.7821 0.8095 29.2621 0.2747 0 0.875 0.875 0 0 0 3 6 29.59418.255 0.8479 30.6516 0.1306 0 0 0 0 0 0 3 7 27.2904 16.7775 0.791628.6165 0.117 0 0 0 0 0 0 3 8 32.0759 21.3168 1.0149 36.687 0.1287 0 0 00 0 0 3 9 11.3167 8.9989 0.3238 11.7044 0.0337 0 0 0 0 0.875 0 3 1047.8794 1.867 0.6668 24.1028 0.5212 0 0.875 0 0 0 0 3 11 38.1087 10.09640.8129 29.3858 0.2958 0 0 0 0 0 0 3 12 29.1087 12.0353 0.731 26.42530.167 0 0 0 0 0 0 3 13 32.9772 21.6736 1.001 36.1859 0.1453 0 0 0 0 0 03 14 26.1774 17.2847 0.7394 26.7277 0.0884 0 0 0 0 0.875 0 3 15 44.01397.4653 0.7942 28.7088 0.4053 0 0.875 0 0 0 0 3 16 3.3654 3.7276 0.04261.5406 −0.0027 0 0 0 0 0 0 4 1 25.492 16.5937 0.7634 27.5979 0.0911 0 00.75 0 0 0 4 2 25.0526 16.4405 0.7271 26.2844 0.0861 0 0 0.75 0 0 0 4 326.6439 16.1513 0.7463 26.977 0.0889 0 0 0.75 0 0 0 4 4 8.939 4.44710.1855 6.7042 0.0195 0 0 0.75 0 0.75 0 4 5 31.3599 14.4563 0.778528.1423 0.1927 0 0.75 0.75 0 0 0 4 6 32.6696 17.1698 0.8987 32.48740.1475 0 0 0 0 0 0 4 7 31.6017 13.1545 0.7725 27.9246 0.1942 0 0 0 0 0 04 8 33.4823 19.718 1.0123 36.5929 0.1326 0 0 0 0 0 0 4 9 12.4995 6.30690.375 13.5551 0.046 0 0 0 0 0.75 0 4 10 48.6152 −4.3375 0.6394 23.1150.5697 0 0.75 0 0 0 0 4 11 42.989 5.7041 0.7377 26.6675 0.3792 0 0 0 0 00 4 12 32.6771 8.7176 0.7127 25.7625 0.245 0 0 0 0 0 0 4 13 35.46414.8498 0.9578 34.6247 0.2053 0 0 0 0 0 0 4 14 24.0107 14.9324 0.7226.0278 0.0894 0 0 0 0 0.75 0 4 15 39.2751 8.6633 0.8092 29.2522 0.319 00.75 0 0 0 0 4 16 31.806 15.0401 0.8979 32.4605 0.1745 0.1275 0 0 0 0 05 1 26.262 16.477 0.7293 26.3635 0.088 0 0 0.625 0 0 0 5 2 23.932315.5571 0.7185 25.9736 0.0827 0 0 0.625 0 0 0 5 3 25.3808 16.1474 0.785728.403 0.0965 0 0 0.625 0 0 0 5 4 9.1171 4.2487 0.2386 8.6247 0.0208 0 00.625 0 0.625 0 5 5 26.6273 17.4591 0.8121 29.3586 0.1114 0 0.625 0.6250 0 0 5 6 32.4494 18.2364 0.8924 32.2599 0.1711 0 0 0 0 0 0 5 7 40.58217.1924 0.6488 23.4554 0.3589 0 0 0 0 0 0 5 8 32.5308 20.5892 0.992235.8668 0.1299 0 0 0 0 0 0 5 9 18.0317 15.0408 0.5278 19.0801 0.0576 0 00 0 0.625 0 5 10 46.3191 0.5778 0.6724 24.3059 0.5198 0 0.625 0 0 0 0 511 44.6369 1.626 0.6829 24.6876 0.4534 0 0 0 0 0 0 5 12 35.4393 5.75060.6467 23.3795 0.3016 0 0 0 0 0 0 5 13 35.4493 21.0168 0.9146 33.06250.189 0 0 0 0 0 0 5 14 27.0781 19.2557 0.7971 28.8141 0.1019 0 0 0 00.625 0 5 15 37.2533 13.087 0.8139 29.4226 0.2787 0 0.625 0 0 0 0 5 163.6561 3.1878 0.0318 1.148 −0.0025 0 0 0 0 0 0 6 1 24.6778 22.03990.7405 26.7684 0.0826 0 0 0.5 0 0 0 6 2 25.2229 17.6846 0.7461 26.97220.0905 0 0 0.5 0 0 0 6 3 25.0098 18.2845 0.7368 26.6363 0.0886 0 0 0.5 00 0 6 4 15.0796 11.334 0.4265 15.4161 0.0468 0 0 0.5 0 0.5 0 6 5 26.444221.9848 0.7821 28.2731 0.0996 0 0.5 0.5 0 0 0 6 6 33.7204 18.2395 0.85430.8704 0.2042 0 0 0 0 0 0 6 7 48.6329 0.1423 0.5077 8.353 0.5727 0 0 00 0 0 6 8 32.9598 20.2321 0.977 35.3184 0.1325 0 0 0 0 0 0 6 9 27.484716.0934 0.809 29.2465 0.1045 0 0 0 0 0.5 0 6 10 47.3126 1.909 0.651123.536 0.5108 0 0.5 0 0 0 0 6 11 44.8464 3.0427 0.6707 24.2472 0.4515 00 0 0 0 0 6 12 38.7726 6.4545 0.5984 21.6335 0.3634 0 0 0 0 0 0 6 1338.5156 3.2083 0.8575 30.9968 0.2641 0 0 0 0 0 0 6 14 28.7859 18.10870.8805 31.8313 0.1271 0 0 0 0 0.5 0 6 15 35.4929 17.1934 0.7562 27.33450.2432 0 0.5 0 0 0 0 6 16 2.5988 1.2055 −0.0164 −0.5943 −0.0095 0 0 0 00 0 7 1 23.6924 16.7271 0.7004 25.3191 0.0826 0 0 0.375 0 0 0 7 225.1267 21.1141 0.7418 26.8149 0.0847 0 0 0.375 0 0 0 7 3 25.895918.4176 0.7671 27.7314 0.0901 0 0 0.375 0 0 0 7 4 18.8393 12.6193 0.534119.3068 0.0639 0 0 0.375 0 0.375 0 7 5 28.357 18.3763 0.8591 31.05550.1054 0 0.375 0.375 0 0 0 7 6 37.6451 12.7384 0.8363 30.2303 0.2795 0 00 0 0 0 7 7 50.5621 −8.9297 0.4671 16.885 0.6403 0 0 0 0 0 0 7 8 32.236419.6481 0.956 34.5605 0.1362 0 0 0 0 0 0 7 9 28.8909 18.0531 0.870131.4548 0.1113 0 0 0 0 0.375 0 7 10 47.559 2.1238 0.5786 20.9158 0.53120 0.375 0 0 0 0 7 11 46.2019 1.1774 0.6161 22.2705 0.4965 0 0 0 0 0 0 712 41.8835 −0.2463 0.5734 20.7288 0.4401 0 0 0 0 0 0 7 13 38.938511.7442 0.8471 30.6208 0.2895 0 0 0 0 0 0 7 14 32.6869 21.8404 0.944134.1293 0.1518 0 0 0 0 0.375 0 7 15 33.6641 15.6957 0.7471 27.007 0.23950 0.375 0 0 0 0 7 16 34.1815 15.6762 0.9132 33.013 0.1882 0.1275 0 0 0 00 8 1 24.3356 15.0031 0.7199 26.0256 0.0889 0 0 0.25 0 0 0 8 2 24.50116.4553 0.7674 27.7415 0.097 0 0 0.25 0 0 0 8 3 26.1797 15.4862 0.775828.0436 0.0977 0 0 0.25 0 0 0 8 4 23.9023 13.5114 0.6887 24.8975 0.08640 0 0.25 0 0.25 0 8 5 27.2773 16.1215 0.8158 29.4917 0.1019 0 0.25 0.250 0 0 8 6 43.6154 1.6883 0.7068 25.5505 0.4304 0 0 0 0 0 0 8 7 54.0389−18.2872 0.2857 10.327 0.768 0 0 0 0 0 0 8 8 32.2327 19.5627 0.911132.9365 0.1482 0 0 0 0 0 0 8 9 29.5791 16.0012 0.8473 30.6296 0.1394 0 00 0 0.25 0 8 10 49.7662 −9.2035 0.5443 19.6769 0.6038 0 0.25 0 0 0 0 811 48.2982 −7.9653 0.5573 20.1458 0.566 0 0 0 0 0 0 8 12 43.5519 −1.56490.5715 20.6589 0.4762 0 0 0 0 0 0 8 13 42.773 7.9963 0.7849 28.37520.3819 0 0 0 0 0 0 8 14 31.8568 17.6636 0.8855 32.0102 0.1807 0 0 0 00.25 0 8 15 35.8667 9.7526 0.7675 27.7441 0.275 0 0.25 0 0 0 0 8 161.3994 3.1514 −0.006 −0.2176 −0.0045 0 0 0 0 0 0 9 1 18.3331 11.06660.5484 19.8255 0.0638 0 0 0.25 0.2 0 0 9 2 22.798 15.9195 0.6977 25.22210.0827 0 0 0.4375 0 0 0 9 3 13.6014 15.3552 0.3517 12.7144 0.0312 0 00.625 0 0 0 9 4 28.351 21.8465 0.8623 31.1733 0.1033 0 0 0.8125 0 0 1 95 29.4335 21.2793 0.9293 33.5925 0.1106 0 1 0 0 0 0 9 6 21.2667 16.57140.5955 21.5278 0.0682 0 0 0 0.2 0 0 9 7 25.3599 18.0756 0.7027 25.4020.0854 0 0 0 0 0 0 9 8 21.966 14.7363 0.6219 22.481 0.0736 0 0 0 0 0 0 99 31.1704 19.4661 0.8974 32.4422 0.1305 0 0 0 0 0 1 9 10 31.8494 19.29230.9109 32.9279 0.1397 0 1 0 0 0 0 9 11 17.0166 13.0969 0.4865 17.58820.051 0 0 0 0.2 0 0 9 12 25.0631 16.8801 0.7186 25.9785 0.0869 0 0 0 0 00 9 13 19.9114 13.2859 0.5459 19.7345 0.0645 0 0 0 0 0 0 9 14 31.520418.4006 0.8541 30.874 0.1476 0 0 0 0 0 1 9 15 34.16 17.1821 0.866131.3099 0.1905 0 0 0 0 0 0 9 16 2.7882 4.2082 0.0005 0.0192 0.0095 0 0 00 0 0 10 1 20.1799 15.6023 0.5626 20.3382 0.0639 0 0 0.25 0.1786 0 0 102 23.8584 16.4225 0.6988 25.2598 0.0823 0 0 0.4375 0 0 0 10 3 15.438811.8361 0.4277 15.4606 0.0438 0 0 0.625 0 0 0 10 4 29.1664 21.68230.8605 31.1062 0.0999 0 0 0.8125 0 0 0.8929 10 3 29.7657 20.4923 0.89332.2799 0.1072 0 0.8929 0 0 0 0 10 6 22.18 16.7809 0.6181 22.3455 0.07090 0 0 0.1786 0 0 10 7 26.8964 18.4335 0.7687 27.7879 0.0978 0 0 0 0 0 010 8 22.7626 17.3084 0.6298 22.7655 0.0704 0 0 0 0 0 0 10 9 31.054120.3764 0.8791 31.7796 0.1285 0 0 0 0 0 0.8929 10 10 31.5314 20.16110.8887 32.1276 0.1379 0 0.8929 0 0 0 0 10 11 18.497 14.278 0.5299 9.15460.054 0 0 0 0.1786 0 0 10 12 27.0928 17.5518 0.777 28.0886 0.1001 0 0 00 0 0 10 13 23.9418 16.8238 0.6968 25.1885 0.0802 0 0 0 0 0 0 10 1432.8367 16.8366 0.8584 31.0301 0.1726 0 0 0 0 0 0.8929 10 15 35.384516.154 0.8552 30.9151 0.2129 0 0.8929 0 0 0 0 10 16 32.4924 16.39730.857 30.9802 0.1675 0.1275 0 0 0 0 0 11 1 17.8706 12.5355 0.539 19.48490.0583 0 0 0.25 0.1571 0 0 11 2 22.1385 14.6388 0.6381 23.0678 0.0756 00 0.4375 0 0 0 11 3 16.2493 9.7877 0.4863 17.5787 0.0511 0 0 0.625 0 0 011 4 28.4408 19.613 0.8619 31.1555 0.1022 0 0 0.8125 0 0 0.7857 11 528.7788 20.3358 0.8639 31.2296 0.1008 0 0.7857 1 0 5 0 11 6 21.334115.2564 0.5892 21.2992 0.0673 0 0 0 0.1571 0 0 11 7 27.2565 17.52950.7991 28.886 0.1046 0 0 0 0 0 0 11 8 22.8741 15.5232 0.6559 23.70950.0754 0 0 0 0 0 0 11 9 31.075 18.1195 0.917 33.1497 0.1331 0 0 0 0 00.7857 11 10 31.3771 18.8457 0.8762 31.6749 0.1522 0 0.7857 0 0 0 0 1111 21.3374 14.1823 0.6491 23.4647 0.0785 0 0 0 0.1571 0 0 11 12 25.525416.7175 0.76 27.4744 0.1037 0 0 0 0 0 0 11 13 20.9039 14.4462 0.6423.1367 0.0754 0 0 0 0 0 0 11 14 33.7178 14.9458 0.8333 30.1232 0.2011 00 0 0 0 0.7857 11 15 34.0506 15.3472 0.8472 30.6271 0.2145 0 0.7857 0 00 0 11 16 0.2666 0.8625 −0.0072 −0.2617 −0.0041 0 0 0 0 0 0 12 1 18.425212.5906 0.6282 22.7083 0.0734 0 0 0.25 0.1357 0 0 12 2 21.4727 15.78980.6968 25.1879 0.0852 0 0 0.4375 0 0 0 12 3 14.1262 12.3376 0.468716.9417 0.0497 0 0 0.625 0 0 0 12 4 26.6361 19.8449 0.8375 30.27510.0896 0 0 0.8125 0 0 0.6786 12 5 26.1247 23.2018 0.7532 27.2264 0.08130 0.6786 1 0 0 0 12 6 25.9088 17.9446 0.7612 27.5175 0.0905 0 0 0 0.13570 0 12 7 25.573 24.4683 0.7131 25.7792 0.0985 0 0 0 0 0 0 12 8 24.26217.1356 0.7712 27.8785 0.0918 0 0 0 0 0 0 12 9 29.8063 15.9041 0.871231.4939 0.1526 0 0 0 0 0 0.6786 12 10 34.0875 13.806 0.859 31.05130.2288 0 0.6786 0 0 0 0 12 11 23.2764 16.0656 0.7007 25.3292 0.0852 0 00 0.1357 0 0 12 12 26.9347 14.5078 0.7474 27.0175 0.115 0 0 0 0 0 0 1213 25.0739 14.2758 0.813 29.3912 0.1076 0 0 0 0 0 0 12 14 34.2818 9.77620.8339 30.1465 0.2607 0 0 0 0 0 0.6786 12 15 35.628 9.6941 0.818129.5727 0.2742 0 0.6786 0 0 0 0 12 16 0.8243 0.262 0.0134 0.4858 0.00250 0 0 0 0 0 13 1 18.3427 17.1145 0.5463 19.7493 0.0541 0 0 0.25 0.1143 00 13 2 21.3958 19.2387 0.599 21.6519 0.063 0 0 0.4375 0 0 0 13 3 15.865613.3135 0.449 16.2312 0.0452 0 0 0.625 0 0 0 13 4 27.8323 18.0095 0.818229.5764 0.0982 0 0 0.8125 0 0 0.5714 13 5 27.6816 18.912 0.8077 29.19840.0936 0 0.5714 1 0 0 0 13 6 26.0154 20.0225 0.8041 29.0693 0.0909 0 0 00.1143 0 0 13 7 27.321 17.8397 0.8275 29.9151 0.1259 0 0 0 0 0 0 13 825.8111 17.8768 0.7658 27.6837 0.0907 0 0 0 0 0 0 13 9 32.5862 15.98160.7969 28.8078 0.1975 0 0 0 0 0 0.5714 13 10 41.3818 4.9336 0.701525.3603 0.3954 0 0.5714 0 0 0 0 13 11 24.8301 17.6776 0.6894 24.92140.0831 0 0 0 0.1143 0 0 13 12 26.8437 15.7759 0.7715 27.8911 0.1353 0 00 0 0 0 13 13 24.7873 17.0919 0.751 27.1481 0.0946 0 0 0 0 0 0 13 1434.4795 12.7622 0.74 26.7515 0.2396 0 0 0 0 0 0.5714 13 15 36.440411.2958 0.7768 28.0793 0.2677 0 0.5714 0 0 0 0 13 16 32.5622 16.82880.7849 28.3746 0.1755 0.1275 0 0 0 0 0 14 1 20.2567 12.3853 0.671224.2633 0.0852 0 0 0.25 0.0929 0 0 14 2 22.68 15.5979 0.7275 26.29960.0862 0 0 0.4375 0 0 0 14 3 7.0763 12.9293 0.5885 21.273 0.0675 0 00.625 0 0 0 14 4 26.0405 18.4515 0.8042 29.07 0.1036 0 0 0.8125 0 00.4643 14 5 26.0927 19.3723 0.7707 27.8589 0.0941 0 0.4643 1 0 0 0 14 624.2827 16.6636 0.7693 27.8114 0.0989 0 0 0 0.0929 0 0 14 7 27.819515.8631 0.8198 29.6364 0.1473 0 0 0 0 0 0 14 8 26.9972 16.5785 0.807629.1956 0.11 0 0 0 0 0 0 14 9 38.8468 6.9959 0.7191 25.9951 0.3418 0 0 00 0 0.4643 14 10 48.9533 4.4406 0.5294 9.1373 0.5957 0 0.4643 0 0 0 0 1411 24.6424 16.8798 0.7738 27.9708 0.1041 0 0 0 0.0929 0 0 14 12 28.140713.399 0.7724 27.9235 0.1621 0 0 0 0 0 0 14 13 27.1547 16.2099 0.759327.4492 0.1341 0 0 0 0 0 0 14 14 36.8809 8.2728 0.6993 25.2804 0.3112 00 0 0 0 0.4643 14 15 36.4174 8.3339 0.7383 26.6874 0.3082 0 0.4643 0 0 00 14 16 1.1257 0.8364 −0.0533 −1.9279 −0.0116 0 0 0 0 0 0 15 1 19.930515.9556 0.6162 22.277 0.071 0 0 0.25 0.0714 0 0 15 2 22.3009 14.33220.743 26.8605 0.0864 0 0 0.4375 0 0 0 15 3 18.8732 13.6249 0.614322.2054 0.0672 0 0 0.625 0 0 0 15 4 24.0558 15.8686 0.7818 28.2606 0.1030 0 0.8125 0 0 3.3571 15 5 25.927 17.3231 0.7769 28.0848 0.0937 0 0.35711 0 0 0 15 6 26.5932 17.8376 0.8142 29.4341 0.1077 0 0 0 0.0714 0 0 15 729.5785 15.1647 0.8206 29.6653 0.2062 0 0 0 0 0 0 15 8 27.0224 17.60580.8195 29.6227 0.1215 0 0 0 0 0 0 15 9 45.5964 −1.427 0.6094 22.0310.5239 0 0 0 0 0 0.3571 15 10 47.7892 −4.8284 0.5902 21.3358 0.5789 03.3571 0 0 0 0 15 11 27.2611 16.2992 0.784 28.3422 0.1126 0 0 0 0.0714 00 15 12 30.9992 12.5497 0.7158 25.8775 0.2007 0 0 0 0 0 0 15 13 31.80539.9612 0.7893 28.5319 0.2159 0 0 0 0 0 0 15 14 37.3824 5.9023 0.739326.7266 0.3762 0 0 0 0 0 0.3571 15 15 38.1161 5.5222 0.698 25.23090.3851 0 0.3571 0 0 0 0 15 16 0.8754 0.7034 −0.0221 −0.7984 −0.0015 0 00 0 0 0 16 1 5.642 6.3495 0.1244 4.4983 0.0117 0 0 0.25 0.05 0 0 16 220.1376 15.5842 0.6325 22.8636 0.0761 0 0 0.4375 0 0 0 16 3 17.7215.0247 0.5638 20.3814 0.0668 0 0 0.625 0 0 0 16 4 20.745 16.5113 0.676824.4663 0.0809 0 0 0.8125 0 0 0.25 16 5 23.4069 16.7755 0.7548 27.28560.0951 0 0.25 1 0 0 0 16 6 28.4013 17.264 0.8013 28.9677 0.1431 0 0 00.05 0 0 16 7 34.7081 11.4293 0.7565 27.3464 0.2707 0 0 0 0 0 0 16 831.5206 15.0594 0.7868 28.4425 0.1976 0 0 0 0 0 0 16 9 50.5474 −10.49830.4745 17.1519 0.6572 0 0 0 0 0 0.25 16 10 53.9071 −15.5894 0.350312.6648 0.7563 0 0.25 0 0 0 0 16 11 28.0202 14.2589 0.7625 27.5636 0.1560 0 0 0.05 0 0 16 12 37.4585 −1.0934 0.6168 22.2983 0.4116 0 0 0 0 0 016 13 38.0537 −0.1529 0.5897 21.3174 0.4244 0 0 0 0 0 0 16 14 43.3047−5.8456 0.4632 16.7442 0.5402 0 0 0 0 0 0.25 16 15 43.8393 −6.24570.4623 16.7117 0.5811 0 0.25 0 0 0 0 16 16 31.5947 17.1493 0.952634.4377 0.162 0.1275 0 0 0 0 0 Tem- pera- ture: SUM_(—) 300 C. micro-mol % mol % R C NH42nOOX2 NH43SbOX3 PtNH32NO22 RhNO33 RuNONO33 SnOX2VOX2 ZrONO32 mols CO Fe real real real real real real real real realreal 1 1 0 0 0 0 0 0 0 0 0.1275 0 0 1 2 0 0 0 0 0 0 0 0 0 0 0 1 3 0 0 00 0 0 0 0 0 0 0 1 4 0 0 0 0 0 0 0 0 0 0 0 1 5 0 0 0 0 0 0 0 0 0 0 0 1 60 0 0 0 0 0 0 0 0 0 0 1 7 0 0 0 0 0 0 0 0 0.1275 0 0 1 8 0 0 0 0 0 0 0 00 0 0 1 9 0 0 0 0 0 0 0 0 0 0 0 1 10 0 0 0 0 0 0 0 0 0 0 0 1 11 0 0 0 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21.7 14.48 0 0 63.82 0 7 14 0 63.82 0 0 0 21.7 14.48 0 0 00 7 15 0 0 0 0 0 21.7 14.48 0 0 0 0 7 16 0 0 0 0 0 100 0 0 0 0 0 8 1 0 00 39.84 0 20.32 0 0 0 0 0 8 2 0 0 0 0 0 20.32 0 0 0 0 39.84 8 3 0 0 0 00 20.32 0 0 0 39.84 0 8 4 0 39.84 0 0 0 20.32 0 0 0 0 0 8 5 0 0 0 0 020.32 0 0 0 0 0 8 6 0 0 0 52.58 0 26.81 0 20.61 0 0 0 8 7 0 0 0 0 026.81 0 20.61 0 0 52.58 8 8 0 0 0 0 0 26.81 0 20.61 0 52.58 0 8 9 052.58 0 0 0 26.81 0 20.61 0 0 0 8 10 0 0 0 0 0 26.81 0 20.61 0 0 0 8 110 0 0 52.66 0 26.86 20.48 0 0 0 0 8 12 0 0 0 0 0 26.86 20.48 0 0 0 32.668 13 0 0 0 0 0 26.86 20.48 0 0 52.66 0 8 14 0 52.66 0 0 0 26.86 20.48 00 0 0 8 15 0 0 0 0 0 26.86 20.48 0 0 0 0 8 16 0 0 0 0 0 0 0 0 0 0 0 9 134.63 0 0 0 0 22.08 0 0 0 0 0 9 2 0 0 0 0 0 16.67 0 0 26.14 0 0 9 3 0 00 0 21 13.39 0 0 0 0 0 9 4 0 0 51.55 0 0 6.57 0 0 0 0 0 9 5 0 0 0 0 05.99 0 0 0 0 0 9 6 56.82 0 0 0 0 36.22 0 6.96 0 0 0 9 7 0 0 0 0 0 36.220 6.96 36.82 0 0 9 8 0 0 0 0 56.82 36.22 0 6.96 0 0 0 9 9 0 0 86.81 0 011.07 0 2.13 0 0 0 9 10 0 0 0 0 0 11.07 0 2.13 0 0 0 9 11 56.85 0 0 0 036.24 6.91 0 0 0 0 9 12 0 0 0 0 0 36.24 6.91 0 56.85 0 0 9 13 0 0 0 056.85 36.24 6.91 0 0 0 0 9 14 0 0 86.82 0 0 11.07 2.11 0 0 0 0 9 15 0 00 0 0 11.07 2.11 0 0 0 0 9 16 0 0 0 0 0 0 0 0 0 0 0 10 1 32.11 0 0 0 022.93 0 0 0 0 0 10 2 0 0 0 0 0 17.15 0 0 24.02 0 0 10 3 0 0 0 0 19.1813.69 0 0 0 0 0 10 4 0 0 48.71 0 0 6.96 0 0 0 0 0 10 5 0 0 0 0 0 6.31 00 0 0 0 10 6 52.36 0 0 0 0 37.38 0 10.26 0 0 0 10 7 0 0 0 0 0 37.38 010.26 52.36 0 0 10 8 0 0 0 0 52.36 37.38 0 10.26 0 0 0 10 9 0 0 84.6 0 012.08 0 3.32 0 0 0 10 10 0 0 0 0 0 12.08 0 3.32 0 0 0 10 11 52.4 0 0 0 037.41 10.19 0 0 0 0 10 12 0 0 0 0 0 37.41 10.19 0 32.4 0 0 10 13 0 0 0 052.4 37.41 10.19 0 0 0 0 10 14 0 0 84.63 0 0 12.08 3.29 0 0 0 0 10 15 00 0 0 0 12.08 3.29 0 0 0 0 10 16 0 0 0 0 0 100 0 0 0 0 0 11 1 29.39 0 00 0 23.85 0 0 0 0 0 11 2 0 0 0 0 0 17.66 0 0 21.76 0 0 11 3 0 0 0 017.28 14.02 0 0 0 0 0 11 4 0 0 45.53 0 0 7.39 0 0 0 0 0 11 5 0 0 0 0 06.66 0 0 0 0 0 11 6 47.6 0 0 0 0 38.62 0 13.78 0 0 0 11 7 0 0 0 0 038.62 0 13.78 47.6 0 0 11 8 0 0 0 0 47.6 38.62 0 13.78 0 0 0 11 9 0 081.95 0 0 13.3 0 4.75 0 0 0 11 10 0 0 0 0 0 13.3 0 4.75 0 0 0 11 1147.65 0 0 0 0 38.66 13.68 0 0 0 0 11 12 0 0 0 0 0 38.66 13.68 0 47.65 00 11 13 0 0 0 0 47.65 38.66 13.68 0 0 0 0 11 14 0 0 11.99 0 0 13.3 4.710 0 0 0 11 15 0 0 0 0 0 13.3 4.71 0 0 0 0 11 16 0 0 0 0 0 0 0 0 0 0 0 121 26.44 0 0 0 0 24.84 0 0 0 0 0 12 2 0 0 0 0 0 18.2 0 0 19.37 0 0 12 3 00 0 0 15.28 14.35 0 0 0 0 0 12 4 0 0 41.92 0 0 7.88 0 0 0 0 0 12 5 0 0 00 0 7.06 0 0 0 0 0 12 6 42.52 0 0 0 0 39.94 0 17.54 0 0 0 12 7 0 0 0 0 039.94 0 17.54 42.52 0 0 12 8 0 0 0 0 42.52 39.94 0 17.54 0 0 0 12 9 0 078.71 0 0 14.79 0 6.5 0 0 0 12 10 0 0 0 0 0 14.79 0 6.5 0 0 0 12 1142.58 0 0 0 0 40 17.42 0 0 0 0 12 12 0 0 0 0 0 40 17.42 0 42.58 0 0 1213 0 0 0 0 42.58 40 17.42 0 0 0 0 12 14 0 0 78.76 0 0 14.8 6.45 0 0 0 012 15 0 0 0 0 0 14.8 6.45 0 0 0 0 12 16 0 0 0 0 0 0 0 0 0 0 0 13 1 23.240 0 0 0 25.93 0 0 0 0 0 13 2 0 0 0 0 0 18.77 0 0 16.82 0 0 13 3 0 0 0 013.19 14.71 0 0 0 0 0 13 4 0 0 37.81 0 0 8.44 0 0 0 0 0 13 5 0 0 0 0 07.5 0 0 0 0 0 13 6 37.07 0 0 0 0 41.36 0 21.57 0 0 0 13 7 0 0 0 0 041.36 0 21.57 37.07 0 0 13 8 0 0 0 0 37.07 41.36 0 21.57 0 0 0 13 9 0 074.65 0 0 16.66 0 8.69 0 0 0 13 10 0 0 0 0 0 16.66 0 8.69 0 0 0 13 1137.14 0 0 0 0 41.43 21.43 0 0 0 0 13 12 0 0 0 0 0 41.43 21.43 0 37.14 00 13 13 0 0 0 0 37.14 41.43 21.43 0 0 0 0 13 14 0 0 74.71 0 0 16.67 8.620 0 0 0 13 15 0 0 0 0 0 16.67 8.62 0 0 0 0 13 16 0 0 0 0 0 100 0 0 0 0 014 1 19.74 0 0 0 0 27.11 0 0 0 0 0 14 2 0 0 0 0 0 19.38 0 0 14.12 0 0 143 0 0 0 0 10.98 15.08 0 0 0 0 0 14 4 0 0 33.06 0 0 9.08 0 0 0 0 0 14 5 00 0 0 0 8.01 0 0 0 0 0 14 6 31.23 0 0 0 0 42.88 0 25.89 0 0 0 14 7 0 0 00 0 42.88 0 25.89 31.23 0 0 14 8 0 0 0 0 31.23 42.88 0 25.89 0 0 0 14 90 0 69.42 0 0 19.06 0 11.51 0 0 0 14 10 0 0 0 0 0 19.06 0 11.51 0 0 0 1411 31.29 0 0 0 0 42.97 25.74 0 0 0 0 14 12 0 0 0 0 0 42.97 25.74 0 31.290 0 14 13 0 0 0 0 31.29 42.97 25.74 0 0 0 0 14 14 0 0 69.49 0 0 19.0811.43 0 0 0 0 14 15 0 0 0 0 0 19.08 11.43 0 0 0 0 14 16 0 0 0 0 0 0 0 00 0 0 15 1 15.91 0 0 0 0 28.4 0 0 0 0 0 15 2 0 0 0 0 0 20.03 0 0 11.22 00 15 0 0 0 0 0 8.67 15.47 0 0 0 0 0 15 4 0 0 27.53 0 0 9.83 0 0 0 0 0 155 0 0 0 0 0 8.59 0 0 0 0 0 15 6 24.94 0 0 0 0 44.51 0 30.55 0 0 0 15 7 00 0 0 0 44.51 0 30.55 24.94 0 0 15 8 0 0 0 0 24.94 44.51 0 30.55 0 0 015 9 0 0 62.42 0 0 22.28 0 15.29 0 0 0 15 10 0 0 0 0 0 22.28 0 15.29 0 00 15 11 25 0 0 0 0 44.63 30.37 0 0 0 0 15 12 0 0 0 0 0 44.63 30.37 0 250 0 15 13 0 0 0 0 25 44.63 30.37 0 0 0 0 15 14 0 0 62.5 0 0 22.31 15.190 0 0 0 15 15 0 0 0 0 T 22.31 15.19 0 0 0 0 15 16 0 0 0 0 0 0 0 0 0 0 016 1 11.7 0 0 0 0 29.82 0 0 0 0 0 16 2 0 0 0 0 0 20.73 0 0 8.13 0 0 16 30 0 0 0 6.23 15.89 0 0 0 0 0 16 4 0 0 21.01 0 0 10.71 0 0 0 0 0 16 5 0 00 0 0 9.26 0 0 0 0 0 16 6 18.15 0 0 0 0 46.28 0 35.57 0 0 0 16 7 0 0 0 00 46.28 0 35.57 18.15 0 0 16 8 0 0 0 0 18.15 46.28 0 35.57 0 0 0 16 9 00 52.58 0 0 26.81 0 20.61 0 0 0 16 10 0 0 0 0 0 26.81 0 20.61 0 0 0 1611 18.2 0 0 0 0 46.41 35.38 0 0 0 0 16 12 0 0 0 0 0 46.41 35.38 0 18.2 00 16 13 0 0 0 0 18.2 46.41 35.38 0 0 0 0 16 14 0 0 52.66 0 0 26.86 20.480 0 0 0 16 15 0 0 0 0 0 26.86 20.48 0 0 0 0 16 16 0 0 0 0 0 100 0 0 0 00 Tem- pera- ture 350 C. Pt1.0%/ R C COCONV H2OCONV CO2PROD CO2PERPRODCH4PROD ZrO2std CONO32 FeNO33 GeOX2 H2MoO4 LaNO33 1 1 26.6121 4.23130.5077 18.1105 0.2508 0.1275 0 0 0 0 0 1 2 0.7229 −0.0412 0.019 0.67860.0037 0 0 0 0 0 0 1 3 0.1711 0.8278 −0.0091 −0.3252 −0.0032 0 0 0 0 0 01 4 −0.908 0.1406 −0.0264 −0.943 −0.0045 0 0 0 0 0 0 1 5 −0.7495 0.836−0.0283 −1.0102 −0.0058 0 0 0 0 0 0 1 6 2.4441 1.7805 0.068 2.42410.0064 0 0 0 0 0 0 1 7 28.9966 3.751 3.6072 21.6574 0.2614 0.1275 0 0 00 0 1 8 2.0242 0.7457 3.0535 1.9071. 0.0052 0 0 0 1 0 0 1 9 2.93434.3874 0.0851 3.0351 0.0069 0 0 0 1 0 0 1 10 0.1488 −0.8318 −0.0195−0.6938 −0.0019 0 0 0 0 0 0 1 11 0.7994 2.1609 0.0017 0.0598 −0.0035 0 00 0 0 0 1 12 −0.632 2.4348 −0.0385 1.3723 0.0098 0 0 0 0 0 0 1 1326.1795 5.988 0.5864 20.9167 0.2146 0.1275 0 0 0 0 0 1 14 0.2602 1.2811−0.0335 1.1961 0.0087 0 0 0 0 0 1 1 15 0.6717 1.2437 0.0382 1.36140.0079 0 0 0 0 0 0 1 16 31.5724 1.824 0.5405 19.2785 0.3239 0.1275 0 0 00 0 2 1 7.0841 15.4021 0.56 19.9736 0.0661 0 0 0 0 0 0 2 2 8.0063 2.98740.5891 21.0139 0.0698 0 0 0 0 0 0 2 3 15.0803 15.251 0.4847 17.28920.0549 0 0 1 0 0 0 2 4 4.4842 8.1302 0.1158 4.1317 0.0078 0 0 1 0 1 0 25 17.2844 12.8567 0.5669 20.2224 0.0786 0 1 1 0 0 0 2 6 25.9509 10.38130.642 22.9003 0.1951 0 0 0 0 0 0 2 7 20.65 11.2507 0.5812 20.7331 0.12760 0 0 0 0 0 2 8 21.4474 12.8711 0.6705 23.9149 0.0945 0 0 0 0 0 0 2 93.6449 1.9165 0.1037 3.6976 0.0136 0 0 0 0 1 0 2 10 34.8724 −0.46650.4245 15.1434 0.4166 0 1 0 0 0 0 2 11 36.7992 −0.2947 0.4115 14.67940.442 0 0 0 0 0 0 2 12 24.1156 6.441 0.4378 15.618 0.2335 0 0 0 0 0 0 213 24.9384 10.9649 0.6234 22.2377 0.1666 0 0 0 0 0 0 2 14 8.5274 4.4390.2624 9.359 0.0342 0 0 0 0 1 0 2 15 28.6142 4.9078 0.5576 19.8878 0.2780 1 0 0 0 0 2 16 −0.9584 −1.5171 −0.0252 −0.8998 −0.0047 0 0 0 0 0 0 3 115.8468 12.4486 0.5471 19.5152 0.0659 0 0 0.875 0 0 0 3 2 15.594716.5628 0.5001 17.8378 0.0533 0 0 0.875 0 0 0 3 3 16.0961 14.7791 0.528118.8373 0.0615 0 0 0.875 0 0 0 3 4 5.17 9.7616 0.1347 4.8032 0.0081 0 00.875 0 0.875 0 3 5 20.5579 12.0007 0.5566 19.8525 0.1333 0 0.875 0.8750 0 0 3 6 26.1452 9.8078 0.655 23.3632 0.192 0 0 0 0 0 0 3 7 23.21988.8504 0.6154 21.9527 0.1619 0 0 0 0 0 0 3 8 21.1574 18.5925 0.670623.9191 0.1001 0 0 0 0 0 0 3 9 3.7143 0.7242 0.1444 5.1504 0.0214 0 0 00 0.875 0 3 10 37.747 −2.5078 0.5026 17.9292 0.4503 0 0.875 0 0 0 0 3 1141.9429 −7.1208 0.4134 14.7469 0.5312 0 0 0 0 0 0 3 12 28.2739 3.70310.437 15.5872 0.3017 0 0 0 0 0 0 3 13 28.3874 10.9515 0.7197 25.67240.1986 0 0 0 0 0 0 3 14 14.9962 10.1421 0.4954 17.6719 0.065 0 0 0 00.875 0 3 15 31.6362 2.8859 0.5904 21.0596 0.3145 0 0.875 0 0 0 0 3 160.0293 0.2006 −0.008 −0.2849 0.0015 0 0 0 0 0 0 4 1 16.427 9.6501 0.566120.1935 0.0728 0 0 0.75 0 0 0 4 2 15.221 15.321 0.5108 18.2185 0.0607 00 0.75 0 0 0 4 3 19.7181 12.3922 0.6592 23.5147 0.0854 0 0 0.75 0 0 0 44 4.1167 5.5585 0.0614 2.1893 0.0054 0 0 0.75 0 0.75 0 4 5 19.391311.2933 0.6021 21.4763 0.1113 0 0.75 0.75 0 0 0 4 6 27.8954 9.99960.6594 23.5204 0.2203 0 0 0 0 0 0 4 7 28.0012 3.3779 0.507 18.08390.2824 0 0 0 0 0 0 4 8 24.0928 14.3242 0.7318 26.1039 0.1243 0 0 0 0 0 04 9 4.3545 6.5735 0.1031 3.6788 0.0119 0 0 0 0 1.75 0 4 10 40.56027.7433 0.3686 13.1472 0.5263 0 0.75 0 0 0 0 4 11 45.3668 11.3176 0.27579.835 0.6384 0 0 0 0 0 0 4 12 34.4061 1.7401 0.3998 14.2626 0.4243 0 0 00 0 0 4 13 33.4356 4.9956 0.5357 19.1077 0.3461 0 0 0 0 0 0 4 14 12.90598.8004 0.4174 14.89 0.0539 0 0 0 0 0.75 0 4 15 30.3742 2.0829 0.56220.0449 0.304 0 0.75 0 0 0 0 4 16 27.3051 3.9656 0.5117 18.253 0.26150.1275 0 0 0 0 0 5 1 15.4631 9.9059 0.5312 18.9484 0.0679 0 0 0.625 0 00 5 2 16.9891 10.757 0.5687 20.2866 0.0731 0 0 0.625 0 0 0 5 3 16.733214.809 0.5628 20.0763 0.069 0 0 0.625 0 0 0 5 4 4.2413 0.5825 0.2027.2068 0.0341 0 0 0.625 0 0.625 0 5 5 16.7368 15.5641 0.5465 19.49240.0764 0 0.625 0.625 0 0 0 5 6 30.7992 5.3754 0.6441 22.9759 0.288 0 0 00 0 0 5 7 36.572 4.5773 0.4586 16.3571 0.4503 0 0 0 0 0 0 5 8 23.895912.2729 0.7452 26.5801 0.1321 0 0 0 0 0 0 5 9 9.1258 9.806 0.292 10.41410.0352 0 0 0 0 0.625 0 5 10 38.9759 9.0948 0.4173 14.8845 0.5028 0 0.6250 0 0 0 5 11 47.8059 17.9847 0.2779 9.9113 0.6935 0 0 0 0 0 0 5 1237.6722 10.2117 0.3922 13.9881 0.4952 0 0 0 0 0 0 5 13 34.0163 4.7530.6191 22.0845 0.3474 0 0 0 0 0 0 5 14 7.6158 3.8697 0.5551 19.79880.0806 0 0 0 0 0.625 0 5 15 31.1363 1.3651 0.6396 22.8149 0.309 0 0.6251 0 1 0 5 16 1.9025 0.6739 0.0833 2.9712 0.0273 0 0 0 0 1 0 6 1 5.93644.2583 0.5857 20.8918 0.093 0 0 0.5 0 0 0 6 2 18.0377 11.8491 0.599621.3885 0.0792 0 0 0.5 0 0 0 6 3 17.8625 13.0739 0.5751 20.5146 0.0724 00 0.5 0 0 0 6 4 10.7849 10.4828 0.3501 12.4871 0.0464 0 0 0.5 0 0.5 0 65 18.9483 8.7248 0.6339 22.6095 0.0918 0 0.5 0.5 0 0 0 6 6 33.76810.2912 0.595 21.2252 0.3567 0 0 0 0 0 0 6 7 43.9136 −16.1328 0.305810.9082 0.6268 0 0 0 0 0 0 6 8 25.2333 8.1653 0.7274 25.9472 0.1604 0 00 0 0 0 6 9 17.5069 7.8926 0.5625 20.0646 0.0883 0 0 0 0 0.5 0 6 1042.0395 −12.6294 0.3696 13.1828 0.5676 0 0.5 0 0 0 0 6 11 48.9676−20.5759 0.2772 9.8873 0.7122 0 0 0 0 0 0 6 12 40.3603 −11.7344 0.287610.2595 0.5687 0 0 0 0 0 0 6 13 39.5785 −5.8188 0.4669 16.6559 0.491 0 00 0 0 0 6 14 18.5952 12.5173 0.5305 19.6377 0.1124 0 0 0 0 0.5 0 6 1531.2707 −0.048 0.5377 19.1788 0.3366 0 0.5 0 0 0 0 6 16 0.5692 −2.74420.0169 0.6011 0.0092 0 0 0 0 0 0 7 1 15.218 11.9748 0.5167 18.43110.0674 0 Q 0.375 0 0 0 7 2 17.8641 5.1677 0.6448 23.0017 0.0851 0 00.375 0 0 0 7 3 18.3448 7.0319 0.6088 21.7175 0.083 0 0 0.375 0 0 0 7 413.1597 6.9002 0.4945 17.6399 0.0686 0 0 0.375 0 0.375 0 7 5 17.83213.2611 0.6496 23.1697 0.0849 0 0.375 0.375 0 0 0 7 6 36.7106 −3.59590.5086 18.1411 0.4655 0 0 0 0 0 0 7 7 45.0444 −18.4827 0.2609 9.30650.6921 0 0 0 0 0 0 7 8 25.6923 5.912 0.6623 23.6238 0.206 0 0 0 0 0 0 79 18.3993 13.9127 0.5841 20.8345 0.091 0 0 0 0 0.375 0 7 10 42.9402−13.492 0.3736 13.3247 0.5939 0 0.375 0 0 0 0 7 11 49.4756 −21.44990.2336 8.3336 0.745 0 0 0 0 0 0 7 12 42.3764 −15.2733 0.2892 10.31670.6089 0 0 0 0 0 0 7 13 41.0073 −7.1255 0.4211 15.0192 0.5327 0 0 0 0 00 7 14 27.4241 5.9611 0.7143 25.4795 0.2158 0 0 0 0 0.375 0 7 15 31.51592.5661 0.5035 17.9597 0.3461 0 0.375 0 0 0 0 7 16 31.7698 0.1665 0.557919.9 0.3385 0.1275 0 0 0 0 0 8 1 14.6976 8.6991 0.5258 18.757 0.0714 0 00.25 0 0 0 8 2 17.3484 13.7848 0.5742 20.4815 5.0721 0 0 0.25 0 0 5 8 317.9657 0.6273 0.6215 22.1693 0.0856 0 0 0.25 0 0 0 8 4 16.4444 12.38970.552 19.6888 0.0736 0 0 0.25 0 0.25 0 8 5 17.419 10.4163 0.5766 20.56810.08 0 0.25 0.25 0 0 0 8 6 41.5525 −8.8902 0.3588 12.7967 0.5577 0 0 0 00 0 8 7 46.476 −17.8531 0.1542 5.499 0.705 0 0 0 0 0 0 8 8 27.24917.0562 0.5925 21.1361 0.2442 0 0 0 0 0 0 8 9 21.3119 8.2213 0.575320.5219 0.1618 0 0 0 0 0.25 0 8 10 44.4371 −18.7895 0.3125 11.14520.6355 0 0.25 0 0 0 0 8 11 49.1009 −22.5282 0.1618 5.7698 0.7568 0 0 0 00 0 8 12 44.4969 −16.8927 0.2149 7.6663 0.663 0 0 0 0 0 0 8 13 45.3275−12.0025 0.3366 12.0053 0.6387 0 0 0 0 0 0 8 14 29.1399 2.7123 0.562620.069 0.2911 0 0 0 0 0.25 0 8 15 34.5782 −4.8769 0.4912 17.5198 0.41310 0.25 0 0 0 0 8 16 1.2743 −2.7008 −0.03 −1.0688 0.0033 0 0 0 0 0 0 9 111.5083 9.3782 0.4088 14.5805 0.0537 0 0 0.25 0.2 0 0 9 2 142047 12.43820.479 17.0871 0.0606 0 0 0.4375 0 0 0 9 3 7.4459 2.7426 0.3219 11.48160.0501 0 0 0.625 0 0 0 9 4 18.0985 9.7764 0.6565 23.4184 0.0918 0 00.8125 0 0 1 9 5 18.9458 14.752 0.6418 22.8938 0.0841 0 0 1 0 0 0 9 613.2875 12.7718 0.4615 16.4614 0.058 0 0 0 0.2 0 0 9 7 16.2231 12.45070.548 19.5489 0.0771 0 0 0 0 0 0 9 8 3.5706 6.213 0.4808 17.1506 0.06520 0 0 0 0 0 9 9 26.4751 4.5935 0.6475 23.0961 0.2217 0 0 0 0 0 1 9 1025.8073 4.7234 0.6083 21.6975 0.2253 0 0 0 0 0 0 9 11 12.4059 6.05390.4331 15.4495 0.0592 0 0 0 0.2 0 0 9 12 15.2726 10.9813 0.5197 18.53770.07 0 0 0 0 0 0 9 13 1.8369 11.4322 0.4085 14.5708 0.0476 0 0 0 0 0 0 914 28.2605 6.3523 0.5242 18.6978 0.2872 0 0 0 0 0 1 9 15 30.6231 5.57920.5352 19.0915 0.3208 0 0 0 0 0 0 9 16 0.0258 4.3078 −0.0052 −0.1849−0.0032 0 0 0 0 0 0 10 1 11.039 6.347 0.4682 16.7007 0.0657 0 0 0.250.1786 0 0 10 2 14.0721 8.8068 0.5481 19.5523 0.0687 0 0 0.4375 0 0 0 103 9.1083 6.5365 0.3113 11.1035 0.0413 0 0 0.625 0 0 0 10 4 17.405611.5802 0.6699 23.8962 0.086 0 0 0.8125 0 0 0.8929 10 5 19.65 9.6020.6818 24.3192 0.091 0 0.8929 1 0 0 0 10 6 14.7232 7.2897 0.5295 18.88850.071 0 0 0 0.1786 0 0 10 7 16.629 8.8331 0.5963 21.2701 0.1079 0 0 0 00 0 10 8 12.7914 7.1486 0.4534 16.1743 0.0625 0 0 0 0 0 0 10 9 25.45465.0826 0.6132 21.8729 0.2292 0 0 0 0 0 0.8929 10 10 25.9503 5.56870.5927 21.1404 0.2288 0 0.8929 0 0 0 0 10 11 12.9761 7.5932 0.448215.9859 0.0563 0 0 0 0.1786 0 0 10 12 17.4082 8.7968 0.5892 21.01730.0984 0 0 0 0 0 0 10 13 15.5878 5.7496 0.5572 19.8751 0.0763 0 0 0 0 00 10 14 31.6303 0.3149 0.5542 19.7675 0.3436 0 0 0 0 0 0.8929 10 1532.0503 1.2431 0.4897 17.4666 0.3696 0 0.8929 0 0 0 0 10 16 27.4557−0.118 0.5274 18.8129 0.2884 0.1275 0 0 0 0 0 11 1 10.1403 4.9198 0.433615.4667 0.0582 0 0 0.25 0.1571 0 0 11 2 13.7097 7.7748 0.5223 18.63140.0638 0 0 0.4375 0 0 0 11 3 8.5048 4.5283 0.37 13.1978 0.0467 0 0 0.6250 0 0 11 4 16.2509 12.108 0.6142 21.9078 0.0675 0 0 0.8125 0 0 0.7857 115 16.5509 10.4361 0.6059 21.6109 0.0803 0 0.7857 1 0 0 0 11 6 12.23487.6726 0.4923 17.5611 0.0647 0 0 0 0.1571 0 0 11 7 17.5853 6.8906 0.615721.961 0.1288 0 0 0 0 0 0 11 8 13.2999 6.9011 0.4531 16.1616 0.0599 0 00 0 0 0 11 9 25.1299 3.7023 0.6186 22.0654 0.2387 0 0 0 0 0 0.7857 11 1027.2335 4.2125 0.599 21.368 0.2451 0 0.7857 0 0 0 0 11 11 14.5681 7.67560.5272 18.8067 0.0658 0 0 0 0.1571 0 0 11 12 17.7691 9.1387 0.589421.0249 0.109 0 0 0 0 0 0 11 13 11.9905 9.478 0.5287 18.8588 0.0673 0 00 0 0 0 11 14 32.4658 0.5299 0.5409 19.2951 0.3667 0 0 0 0 0 0.7857 1115 31.0779 −2.3001 0.5845 20.8507 0.3615 0 0.7857 0 0 0 0 11 16 −1.4274−2.7581 −0.0222 −0.7901 −0.0036 0 0 0 0 0 0 12 1 10.5005 7.0853 0.426215.2036 0.0532 0 0 0.25 0.1357 0 0 12 2 14.616 9.2859 0.5208 18.57520.0665 0 0 0.4375 0 0 0 12 3 9.3877 5.3689 0.3591 12.8089 0.0491 0 00.625 0 0 0 12 4 18.0691 11.774 0.5965 21.2757 0.0781 0 0 0.8125 0 00.6786 12 5 15.9035 10.5955 0.6116 21.8157 0.0787 0 0.6786 1 0 0 0 12 614.756 9.9956 0.5711 20.3722 0.0775 0 0 0 0.1357 0 0 12 7 20.3739 8.7070.5664 20.2045 0.1421 0 0 0 0 0 0 12 8 16.347 8.9824 0.5447 19.42950.0732 0 0 0 0 0 0 12 9 26.4262 2.5268 0.6155 21.954 0.266 0 0 0 0 00.6786 12 10 32.3702 1.4648 0.5289 18.8656 0.3522 0 0.6786 0 0 0 0 12 1114.1759 7.667 0.5381 19.1932 0.0687 0 0 0 0.1357 0 0 12 12 19.41686.3148 0.5762 20.5532 0.1561 0 0 0 0 0 0 12 13 14.4741 9.2631 0.592821.1456 0.0835 0 0 0 0 0 0 12 14 35.5131 5.175 0.4422 15.7744 0.4338 0 00 0 0 0.6786 12 15 33.8652 6.1037 0.509 18.1547 0.4315 0 0.6786 0 0 0 012 16 0.3858 2.0916 0.0112 0.398 0.0016 0 0 0 1 0 0 13 1 11.1671 7.38840.4586 16.3567 0.0576 0 0 0.25 0.1143 0 0 13 2 13.435 9.2774 0.518518.4945 0.0645 0 0 0.4375 0 0 0 13 3 11.9785 9.0053 0.3386 2.0795 0.04030 0 0.625 0 0 0 13 4 14.153 0.5741 0.5433 9.3784 0.0715 0 0 0.8125 0 00.5714 13 5 15.2108 8.5049 0.5839 20.8267 0.0788 0 0.5714 0 0 0 0 13 614.7554 0.004 0.52 8.5488 0.0691 0 0 0 0.1143 0 0 13 7 19.502 9.7460.5025 17.9225 0.1191 0 0 0 0 0 0 13 8 14.8409 10.3532 0.4943 17.63240.0585 0 0 0 0 0 0 13 9 28.9082 1.206 0.5722 20.4092 0.3106 0 0 0 0 00.5714 13 10 35.8084 5.3825 0.4505 16.0704 0.4498 0 0.5714 0 0 0 0 13 1114.6795 8.1249 0.5794 20.6688 0.0744 0 0 0 0.1143 0 0 13 12 19.67177.3227 0.5748 20.5039 0.1409 0 0 0 0 0 0 13 13 6.5111 0.606 0.52658.7799 0.0613 0 0 0 0 0 0 13 14 30.947 −1.2122 0.5206 18.5702 0.3807 0 00 0 0 0.5714 13 15 31.9566 −2.8864 0.532 18.975 0.4049 0 0.5714 0 0 0 013 16 26.9067 0.2947 0.5181 18.4823 0.3005 0.1275 0 0 0 0 0 14 1 10.51496.8603 0.449 16.0155 0.0561 0 0 0.25 0.0929 0 0 14 2 14.7047 10.38560.5025 17.9226 0.0608 0 0 0.4375 0 0 0 14 3 9.0093 8.1848 0.3854 13.7460.049 0 0 0.625 0 0 0 14 4 13.8408 9.9148 0.5411 19.3028 0.0666 5 00.8125 0 0 0.4643 14 5 15.1176 10.598 0.5468 19.5044 0.0622 0 0.4643 1 00 0 14 6 13.6028 11.5495 0.5007 17.8614 0.0573 0 0 0 0.0929 0 0 14 720.7472 6.2939 0.5791 20.6553 0.1856 0 0 0 0 0 0 14 8 15.444 8.91890.5617 20.0343 0.0721 0 0 0 0 0 0 14 9 34.665 −6.9765 0.4234 15.10280.4607 0 0 0 0 0 0.4643 14 10 41.8002 −12.2274 0.2463 8.7869 0.588 00.4643 0 0 0 0 14 11 16.189 11.8272 0.456 16.2648 0.0607 0 0 0 0.0929 00 14 12 20.3728 6.4137 0.5112 18.2357 0.1689 0 0 0 0 0 0 14 13 16.27489.4744 0.5214 18.5997 0.0929 0 0 0 0 0 0 14 14 33.112 −4.8579 0.42115.016 0.4029 0 0 0 0 0 0.4643 14 15 29.8884 −3.2017 0.4765 16.99770.3685 0 0.4643 0 0 0 0 14 16 −2.8145 −3.2408 −0.0324 −1.1548 −0.0007 00 0 0 0 0 15 1 13.6193 8.337 0.4666 16.6454 0.0526 0 0 0.25 0.0714 0 013 2 13.5502 9.8693 0.5075 18.1036 0.0546 0 0 0.4375 0 0 0 15 3 10.62538.1911 0.3709 13.2302 0.0422 0 0 0.625 0 0 0 15 4 12.8991 9.5828 0.514918.3665 0.0614 0 0 0.8125 0 0 0.3571 15 5 14.1788 10.2878 0.5371 19.15670.057 0 0.3571 1 0 0 0 15 6 15.9106 10.2565 0.5234 18.6704 0.0731 0 0 00.0714 0 0 15 7 25.1361 4.5535 0.5339 19.0451 0.246 0 0 0 0 0 0 15 817.3005 10.5653 0.5725 20.4196 0.0858 0 0 0 0 0 0 15 9 39.3304 −11.60550.3576 12.7543 0.5601 0 0 0 0 0 0.3571 15 10 40.8823 −12.3612 0.314211.209 0.5896 0 0.3571 0 0 0 0 15 11 15.7257 8.0321 0.5488 19.57730.0844 0 0 0 0.0714 0 0 15 12 22.0656 1.9917 0.5208 18.5758 0.2347 0 0 00 0 0 15 13 22.8741 2.8364 0.4776 17.0345 0.2124 0 0 0 0 0 0 15 1434.2248 −5.0631 0.374 13.3415 0.4307 0 0 0 0 0 0.3571 15 15 33.8977−5.8869 0.4112 14.666 0.4412 0 0.3571 0 0 0 0 15 16 1.3407 −2.20660.0002 0.0063 −0.0076 0 0 0 0 0 0 16 1 3.7052 3.6884 0.2144 7.64820.0245 0 0 0.25 0.05 0 0 16 2 8.3106 4.9877 0.3432 12.2412 0.0346 0 00.4375 0 0 0 16 3 6.1593 3.1092 0.3153 11.2457 0.0373 0 0 0.625 0 0 0 164 7.5088 5.7052 0.3146 11.2232 0.0292 0 0 0.8125 0 0 0.25 16 5 11.86765.6885 0.4363 15.5639 0.0542 0 0.25 1 0 0 0 16 6 15.1336 5.6469 0.560419.9894 0.1525 0 0 0 0.05 0 0 16 7 27.5593 −2.1028 0.5175 18.4575 0.31540 0 0 0 0 0 16 8 23.5404 3.2796 0.5291 18.8719 0.2067 0 0 0 0 0 0 16 942.6335 −18.8531 0.2745 9.792 0.6582 0 0 0 0 0 0.25 16 10 44.5777−22.1602 0.2137 7.6209 0.6973 0 0.25 0 0 0 0 16 11 19.465 3.5806 0.571820.3966 0.1768 0 0 0 0.05 0 0 16 12 31.6446 −9.6125 0.3109 11.08970.4374 0 0 0 0 0 0 16 13 29.2167 −9.3215 0.3039 10.8415 0.4154 0 0 0 0 00 16 14 28.5935 −9.8595 0.2779 9.9111 0.4188 0 0 0 0 0 0.25 16 1529.7075 −8.4891 0.2937 10.4778 0.4438 0 0.25 0 0 0 0 16 16 23.66524.1211 0.6603 23.552 0.2043 0.1275 0 0 0 0 0 Tem- pera- ture: SUM_(—)350 C. micro- mol % mol % R C NH42TiOOX2 NH43Sb0X3 PtNH32NO22 RhNO33RuNONO33 SnOX2 VOX2 ZrONO32 mol CO Fe 1 1 0 0 0 0 0 0 0 0 0.1275 0 0 1 20 0 0 0 0 0 0 0 0 0 0 1 3 0 0 0 0 0 0 0 0 0 0 0 1 4 0 0 0 0 0 0 0 0 0 00 1 5 0 0 0 0 0 0 0 0 0 0 0 1 6 0 0 0 0 0 0 0 0 0 0 0 1 7 1 1 0 0 0 0 00 0.1275 0 0 1 8 1 1 0 0 0 0 0 0 0 0 0 1 9 0 0 0 0 0 0 0 0 0 0 0 1 10 00 0 0 0 0 0 0 0 0 0 1 11 0 0 0 0 0 0 0 0 0 0 0 1 12 0 0 0 0 0 0 0 0 0 00 1 13 0 0 0 0 0 0 0 0 0.1275 0 0 1 14 0 0 0 0 0 0 0 0 0 0 0 1 15 0 0 00 0 0 0 0 0 0 0 1 16 0 0 0 0 0 0 0 0 0.1275 0 0 2 1 0 0 0.1275 0 0 0 0 02.1275 0 47 2 2 0 0 0.1275 0 0 0 0 1 2.1275 0 47 2 3 0 0 0.1275 0 0 0 10 2.1275 0 47 2 4 0 0 0.1275 0 0 0 0 0 2.1275 0 47 2 5 0 0 0.1275 0 0 00 0 2.1275 47 47 2 6 1 0 0.1275 0 0.0245 0 0 0 1.152 0 0 2 7 0 0 0.12750 0.0245 0 0 1 1.152 0 0 2 8 0 0 0.1275 0 0.0245 0 1 0 1.152 0 0 2 9 0 00.1275 0 0.0245 0 0 0 1.152 0 0 2 10 0 0 0.1275 0 0.0245 0 0 0 1.15286.81 0 2 11 1 0 0.1275 0.0243 0 0 0 0 1.1518 0 0 2 12 0 0 0.1275 0.02430 V 0 1 1.1518 0 0 2 13 0 0 0.1275 3.0243 0 0 1 0 1.1518 0 0 2 14 0 00.1275 0.0243 0 0 0 0 1.1518 0 0 2 15 0 0 0.1275 0.0243 0 0 0 0 1.151886.82 0 2 16 0 0 0 0 0 0 0 0 0 0 0 3 1 0.875 0 0.1275 0 0 0 0 0 1.8775 046.6 3 2 0 0 0.1275 0 0 0 0 0.875 1.8775 0 46.6 3 3 0 0 0.1275 0 0 00.875 0 1.8775 0 46.6 3 4 0 0 0.1275 0 0 0 0 0 1.8775 0 46.6 3 5 0 00.1275 0 0 0 0 0 1.8775 46.6 46.6 3 6 0.875 0 0.1275 0 0.0368 0 0 01.0393 0 0 3 7 0 0 0.1275 0 0.0368 0 0 0.875 1.0393 0 0 3 8 0 0 0.1275 00.0368 0 0.875 0 1.0393 0 0 3 9 0 0 0.1275 0 0.0368 0 0 0 1.0393 0 0 310 0 0 0.1275 0 0.0368 0 0 0 1.0393 84.2 0 3 11 0.875 0 0.1275 0.0365 00 0 0 1.039 0 0 3 12 0 0 0.1275 0.0365 0 0 0 0.875 1.039 0 0 3 13 0 00.1275 0.0365 0 0 0.875 0 1.039 0 0 3 14 0 0 3.1275 3.0365 0 0 0 0 1.0390 0 3 15 0 0 0.1275 0.0365 0 0 0 0 1.039 84.22 0 3 16 0 0 0 0 0 0 0 0 00 0 4 1 0.75 0 0.1275 0 0 0 0 0 1.6275 0 46.08 4 2 0 0 0.1275 0 0 0 00.75 1.6275 0 46.08 4 3 0 0 0.1275 0 0 0 0.75 0 1.6275 0 46.08 4 4 0 03.1275 0 0 0 0 0 1.6275 0 46.08 4 5 0 0 0.1275 0 0 0 0 0 1.6275 46.0846.08 4 6 0.75 0 0.1275 0 0.049 0 0 0 0.9265 0 0 4 7 0 0 0.1275 0 0.0490 0 0.75 0.9265 0 0 4 8 0 0 0.1275 0 0.049 0 0.75 0 0.9265 0 0 4 9 0 13.1275 0 0.049 0 0 0 0.9265 0 0 4 10 0 0 0.1275 0 0.049 0 0 0 0.926580.95 0 4 11 0.75 0 0.1275 0.0486 0 0 0 0 0.9261 0 0 4 12 0 0 0.12750.0486 0 0 0 0.75 0.9261 0 0 4 13 0 0 0.1275 0.0486 0 0 0.75 0 0.9261 00 4 14 0 0 0.1275 0.0486 0 0 0 0 0.9261 0 0 4 15 0 0 0.1275 0.0486 0 0 00 0.9261 80.98 0 4 16 0 0 0 0 0 0 0 0 0.1275 0 0 5 1 0.625 0 0.1275 0 00 0 0 1.3775 0 45.37 5 2 0 0 0.1275 0 0 0 0 0.625 1.3775 0 45.37 5 3 0 00.1275 0 0 0 0.625 0 1.3775 0 45.37 5 4 0 0 0.1275 0 0 0 0 0 1.3775 045.37 5 5 0 0 0.1275 0 0 0 0 0 1.3775 45.37 45.37 5 6 0.625 0 0.1275 00.0613 0 0 0 0.8138 0 0 5 7 0 0 0.1275 0 0.0613 0 0 0.625 0.8138 0 0 5 80 0 0.1275 0 0.0613 0 0.625 0 0.8138 0 0 5 9 0 0 0.1275 0 0.0613 0 0 00.8138 0 0 5 10 0 0 0.1275 0 0.0613 0 0 0 0.8138 76.8 0 5 11 0.625 00.1275 0.0608 0 0 0 0 0.8133 0 0 5 12 0 0 0.1275 0.0608 0 0 0 0.6250.8133 0 0 5 13 0 0 0.1275 0.0608 0 0 0.625 0 0.8133 0 0 5 14 0 0 0.12750.0608 0 0 0 0 0.8133 0 0 5 15 0 0 3.1275 1.0608 0 1 1 0 1.8133 76.85 05 16 0 0 0 0 0 0 0 0 0 1 0 6 1 0.5 0 0.1275 0 0 0 1 0 1.1275 0 44.35 6 20 0 0.1275 0 0 0 0 0.5 1.1275 0 44.35 6 3 0 0 0.1275 0 0 0 0.5 0 1.12750 44.35 6 4 0 0 0.1275 0 0 0 0 0 1.1275 0 44.35 6 5 0 0 0.1275 0 0 0 0 01.1275 44.35 44.35 6 6 0.5 0 0.1275 0 0.0735 0 0 0 0.701 0 0 6 7 0 00.1275 0 0.0735 0 0 0.5 0.701 0 0 6 8 0 0 0.1275 0 0.0735 0 0.5 0 0.7010 0 6 9 0 0 0.1275 0 0.0735 0 0 0 0.701 0 0 6 10 0 0 0.1275 0 0.0735 0 00 0.701 71.33 0 6 11 0.5 0 0.1275 0.0729 0 0 0 0 0.7004 0 0 6 12 0 00.1275 0.0729 0 0 0 0.5 0.7004 0 0 6 13 0 0 0.1275 0.0729 0 0 0.5 00.7004 0 0 6 14 0 0 0.1275 0.0729 0 0 0 0 0.7004 0 0 6 15 0 0 0.12750.0729 0 0 0 0 0.7004 71.39 0 6 16 0 0 0 0 0 0 0 0 0 0 0 7 1 0.375 00.1275 0 0 0 0 0 0.8775 0 42.74 7 2 0 0 0.1275 0 0 0 0 0.375 0.8775 042.74 7 3 0 0 0.1275 0 0 0 0.375 0 0.8775 0 42.74 7 4 0 0 0.1275 0 0 0 00 0.8775 0 42.74 7 5 0 0 0.1275 0 0 0 0 0 0.8775 42.74 42.74 7 6 0.375 50.1275 5 5.0858 0 0 0 0.5883 0 0 7 7 0 0 0.1275 0 0.0858 0 0 0.3750.5883 0 0 7 8 0 0 0.1275 0 0.0858 0 0.375 0 0.5883 0 0 7 9 0 0 0.1275 00.0858 0 0 0 0.5883 0 0 7 10 0 0 0.1275 0 0.0858 0 0 0 0.5883 63.75 0 711 0.375 0 0.1275 0.0851 0 0 0 0 0.5876 0 0 7 12 0 0 0.1275 0.0851 0 0 00.375 0.5876 0 0 7 13 0 0 0.1275 0.0851 0 0 0.375 0 0.5876 0 0 7 14 0 00.1275 0.0851 0 0 0 0 0.5876 0 0 7 15 0 0 0.1275 0.0851 0 0 0 0 0.587663.82 0 7 16 0 0 0 0 0 0 0 0 0.1275 0 0 8 1 0.25 0 0.1275 0 0 0 0 00.6275 0 39.84 8 2 0 0 5.1275 0 0 0 0 0.25 0.6275 0 39.84 8 3 0 0 0.12750 0 0 0.25 0 0.6275 0 39.84 8 4 0 0 0.1275 0 0 0 0 0 0.6275 0 39.84 8 50 0 0.1275 0 0 0 0 0 0.6275 39.84 39.84 8 6 0.25 0 0.1275 0 0.098 0 0 00.4755 0 0 8 7 0 0 0.1275 0 0.098 0 0 0.25 0.4755 0 0 8 8 0 0 0.1275 00.098 0 0.25 0 0.4755 0 0 8 9 0 0 0.1275 0 0.098 0 0 0 0.4755 0 0 8 10 00 0.1275 0 0.098 0 0 0 0.4755 52.58 0 8 11 0.25 0 0.1275 0.0972 0 0 0 00.4747 0 0 8 12 0 0 0.1275 0.0972 0 0 0 0.25 0.4747 0 0 8 13 0 0 0.12750.0972 0 0 0.25 0 0.4747 0 0 8 14 0 0 0.1275 0.0972 0 0 0 0 0.4747 0 0 815 0 0 0.1275 0.0972 0 0 0 0 0.4747 52.66 0 8 16 0 0 0 0 0 0 0 0 0 0 0 91 0 0 0.1275 0 0 0 0 0 0.5775 0 43.29 9 2 0 0 0.1275 0 0 0.2 0 0 0.765 057.19 9 3 0 0.2 0.1275 0 0 0 0 0 0.9525 0 65.62 9 4 0 0 0.1275 0 0 0 0 01.94 0 41.88 9 5 0 0 0.1275 0 0 0 0 0 2.1275 47 47 9 6 0 0 0.1275 00.0245 0 0 0 0.352 0 0 9 7 0 0 0.1275 0 0.0245 0.2 0 0 0.352 0 0 9 8 00.2 0.1275 0 0.0245 0 0 0 0.352 0 0 9 9 0 0 0.1275 0 0.0245 0 0 0 1.1520 0 9 10 0 0 0.1275 0 1.0245 0 0 0 1.152 86.81 0 9 11 0 0 0.1275 0.02430 0 0 0 0.3518 0 0 9 12 0 0 0.1275 0.0243 0 0.2 0 0 0.3518 0 0 9 13 00.2 0.1275 0.0243 0 0 0 0 0.3518 0 0 9 14 0 0 0.1275 0.0243 0 0 0 01.1518 0 0 9 15 0 0 0.1275 0.0243 0 0 0 0 1.1518 86.82 0 9 16 0 0 0 0 00 0 0 0. 0 0 10 1 0 0 0.1275 0 0 0 0 0 0.5561 0 44.96 10 2 0 0 0.1275 00 0.1786 0 0 0.7436 0 58.84 10 3 0 0.1786 0.1275 0 0 0 0 0 0.9311 067.13 10 4 0 0 0.1275 0 0 0 0 0 1.8329 0 44.33 10 5 0 0 0.1275 0 0 0 0 02.0204 44.19 49.5 10 6 0 0 0.1275 0 0.035 0 0 0 0.3411 0 0 10 7 0 00.1275 0 0.035 0.1786 0 0 0.3411 0 0 10 8 0 0.1786 0.1275 0 0.035 0 0 00.3411 0 0 10 9 0 0 0.1275 0 0.035 0 0 0 1.0554 0 0 10 10 0 0 0.1275 00.035 0 0 0 1.0554 84.6 0 10 11 0 0 0.1275 0.0347 0 0 0 0 0.3408 0 0 1012 0 0 0.1275 3.0347 0 3.1786 0 0 3.3408 0 0 10 13 0 0.1786 0.12750.0347 0 0 0 0 0.3408 0 0 10 14 0 0 0.1275 0.0347 0 0 0 0 1.0551 0 0 1015 0 0 0.1275 0.0347 0 0 0 0 1.0551 84.63 0 10 16 0 0 0 0 0 0 0 0 0.12750 0 11 1 0 0 0.1275 0 0 0 0 0 0.5346 0 46.76 11 2 0 0 0.1275 0 0 0.15710 0 0.7221 0 60.58 11 3 0 0.1571 0.1275 0 0 0 0 0 0.9096 0 68.71 11 4 00 0.1275 0 0 0 0 0 1.7257 0 47.08 11 5 0 0 0.1275 0 0 0 0 0 1.9132 41.0752.27 11 6 0 0 0.1275 0 0.0455 0 0 0 0.3301 0 0 11 7 0 0 0.1275 0 0.04550.1571 0 0 0.3301 0 0 11 8 0 0.1571 0.1275 0 0.0455 0 0 0 0.3301 0 0 119 0 0 0.1275 0 0.0455 0 0 0 0.9587 0 0 11 10 0 0 0.1275 0 0.0455 0 0 00.9587 81.95 0 11 11 0 0 0.1275 0.0451 0 0 0 0 0.3298 0 0 11 12 0 00.1275 0.0451 0 0.1571 0 0 0.3298 0 0 11 13 0 0.1571 0.1275 0.0451 0 0 00 0.3298 0 0 11 14 0 0 0.1275 0.0451 0 0 0 0 0.9583 0 0 11 15 0 0 0.12750.0451 0 0 0 0 3.9583 81.99 0 11 16 0 0 0 0 0 0 0 0 0 0 0 12 1 0 00.1275 0 0 0 0 0 0.5132 0 48.71 12 2 0 0 0.1275 0 0 0.1357 0 0 0.7007 062.44 12 3 0 0.1357 0.1275 0 0 0 0 0 0.8882 0 70.37 12 4 0 0 0.1275 0 00 0 0 1.6186 0 50.2 12 5 0 0 0.1275 0 0 0 0 0 1.8061 37.57 55.37 12 6 00 0.1275 0 0.056 0 0 0 0.3192 0 0 12 7 0 0 0.1275 0 0.056 0.1357 0 00.3192 0 0 12 8 0 0.1357 0.1275 0 0.056 0 0 0 0.3192 0 0 12 9 0 0 0.12750 0.056 0 0 0 0.8621 0 0 12 10 0 0 0.1275 0 0.056 0 0 0 0.8621 78.71 012 11 0 0 0.1275 0.0555 0 0 0 0 0.3188 0 0 12 12 0 0 0.1275 0.0555 00.1357 0 0 0.3188 0 0 12 13 0 0.1357 0.1275 0.0555 0 0 0 0 0.3188 0 0 1214 0 0 0.1275 0.0555 0 0 0 0 0.8616 0 0 12 15 0 0 0.1275 0.0555 0 0 0 00.8616 78.76 0 12 16 0 0 0 0 0 0 0 0 0 0 0 13 1 0 0 0.1275 0 0 0 0 00.4918 0 50.84 13 2 0 0 0.1275 0 0 0.1143 0 0 0.6793 0 64.41 13 3 00.1143 0.1275 0 0 0 0 0 0.8668 0 72.11 13 4 0 0 0.1275 0 0 0 0 0 1.51140 53.76 13 5 0 0 0.1275 0 0 0 0 0 1.6989 33.63 58.86 13 6 0 0 0.1275 00.0665 0 0 0 0.3083 0 0 13 7 0 0 0.1275 0 0.0665 0.1143 0 0 0.3083 0 013 8 0 0.1143 0.1275 0 0.0665 0 0 0 0.3083 0 0 13 9 0 0 0.1275 0 0.06650 0 0 0.7654 0 0 13 10 0 0 0.1275 0 0.0665 0 0 0 0.7654 74.65 0 13 11 00 0.1275 0.066 0 0 0 0 0.3077 0 0 13 12 0 0 0.1275 0.066 0 0.1143 0 00.3077 0 0 13 13 0 0.1143 0.1275 0.066 0 0 0 0 0.3077 0 0 13 14 0 00.1275 0.066 0 0 0 0 0.7649 0 0 13 15 0 0 0.1275 0.066 0 0 0 0 0.764974.71 0 13 16 0 0 0 0 0 0 0 0 0.1275 0 0 14 1 0 0 0.1275 0 0 0 0 00.4704 0 53.15 14 2 0 0 0.1275 0 0 0.0929 0 0 0.6579 0 66.5 14 3 00.0929 0.1275 0 0 0 0 0 0.8454 0 73.93 14 4 0 0 0.1275 0 0 0 0 0 1.40430 57.86 14 5 0 0 0.1275 0 0 0 0 0 1.5918 29.17 62.82 14 6 0 0 0.1275 00.077 0 0 0 0.2974 0 0 14 7 0 0 0.1275 0 0.077 0.0929 0 0 0.2974 0 0 148 0 0.0929 0.1275 0 0.077 0 0 0 0.2974 0 0 14 9 0 0 0.1275 0 0.077 0 0 00.6688 0 0 14 10 0 0 0.1275 0 0.077 0 0 0 0.6688 69.42 0 14 11 0 00.1275 0.0764 0 0 0 0 0.2967 0 0 14 12 0 0 0.1275 0.0764 0 0.0929 0 00.2967 0 0 14 13 0 0.0929 0.1275 0.0764 0 0 0 0 0.2967 0 0 14 14 0 00.1275 0.0764 0 0 2 0 0.6682 0 0 14 15 0 0 0.1275 0.0764 0 0 0 0 0.668269.49 0 14 16 0 0 0 0 0 0 0 0 0 0 0 15 1 0 0 0.1275 0 0 0 0 0 0.4489 055.69 13 2 0 0 0.1275 0 0 0.0714 0 0 0.6364 0 68.74 15 3 0 0.0714 0.12750 0 0 0 0 0.8239 0 75.86 15 4 0 0 0.1275 0 0 0 0 0 1.2971 0 62.64 15 5 00 0.1275 0 0 0 0 0 1.4846 24.06 67.36 15 6 0 0 0.1275 0 0.0875 0 0 00.2864 0 0 15 7 0 0 0.1275 0 0.0875 0.0714 0 0 0.2864 0 0 15 8 0 0.07140.1275 0 0.0875 0 0 0 0.2864 0 0 15 9 0 0 0.1275 0 0.0875 0 0 0 0.5721 00 15 10 0 0 0.1275 0 0.0875 0 0 0 0.5721 62.42 0 15 11 0 0 0.1275 0.08680 0 0 0 0.2857 0 0 15 12 0 0 0.1275 0.0868 0 0.0714 0 0 0.2857 0 0 15 130 0.0714 0.1275 0.0868 0 0 0 0 0.2857 0 0 15 14 0 0 0.1275 0.0868 0 0 00 0.5714 0 0 15 15 0 0 0.1275 0.0868 0 0 0 0 0.5714 62.5 0 15 16 0 0 0 00 0 0 0 0 0 0 16 1 0 0 0.1275 0 0 0 0 0 0.4275 0 58.48 16 2 0 0 0.1275 00 0.05 0 0 0.615 0 71.14 16 3 0 0.05 0.1275 0 0 0 0 0 0.8025 0 77.88 164 0 0 0.1275 0 0 0 0 0 1.19 0 68.28 16 5 0 0 0.1275 0 0 0 0 0 1.377518.15 72.6 16 6 0 0 0.1275 0 0.098 0 0 0 0.2755 0 0 16 7 0 0 0.1275 00.098 0.05 0 0 0.2755 0 0 16 8 0 0.05 0.1275 0 0.098 0 0 0 0.2755 0 0 169 0 0 0.1275 0 0.098 0 0 0 0.4755 0 0 16 10 0 0 0.1275 0 0.098 0 0 00.4755 52.58 0 16 11 0 0 0.1275 0.0972 0 0 0 0 0.2747 0 0 16 12 0 00.1275 0.0972 0 0.05 0 0 0.2747 0 0 16 13 0 0.05 0.1275 0.0972 0 0 0 00.2747 0 0 16 14 0 0 0.1275 0.0972 0 0 0 0 0.4747 0 0 16 15 0 0 0.12750.0972 0 0 0 0 0.4747 52.66 0 16 16 0 0 0 0 0 0 0 0 0.4275 0 0 Tem-pera- ture: 350 C. mol % mol % mol % mol % mol % mol % mol % mol % mol %mol % mol % R C Ge M0 La n Sb Pt Rh Ru Sn V Zr 1 1 0 0 0 0 0 100 0 0 0 00 1 2 0 0 0 0 0 0 0 0 0 0 0 1 3 0 0 0 0 0 0 0 0 0 0 0 1 4 0 0 0 0 0 0 00 0 0 0 1 5 0 0 0 0 0 0 0 0 0 0 0 1 6 0 0 0 0 0 0 0 0 0 0 0 1 7 0 0 0 00 100 0 0 0 0 0 1 8 0 0 0 0 0 0 0 0 0 0 0 1 9 0 0 0 0 0 0 0 0 0 0 0 1 100 0 0 0 0 0 0 0 0 0 0 1 11 0 0 0 0 0 0 0 0 0 0 0 1 12 0 0 0 0 0 0 0 0 00 0 1 13 0 0 0 0 0 100 0 0 0 0 0 1 14 0 0 0 0 0 0 0 0 0 0 0 1 15 0 0 0 00 0 0 0 0 0 0 1 16 0 0 0 0 0 100 0 0 0 0 0 2 1 0 0 0 47 0 5.99 0 0 0 0 02 2 0 0 0 0 0 5.99 0 0 0 0 47 2 3 0 0 0 0 0 5.99 0 0 0 47 0 2 4 0 47 0 00 5.99 0 0 0 0 0 2 5 0 0 0 0 0 5.99 0 0 0 0 0 2 6 0 0 0 86.81 0 11.07 02.13 0 0 0 2 7 0 0 0 0 0 11.07 0 2.13 0 0 86.81 2 8 0 0 0 0 0 11.07 02.13 0 86.81 0 2 9 0 86.81 0 0 0 11.07 0 2.13 0 0 0 2 10 0 0 0 0 0 11.070 2.13 0 0 0 2 11 0 0 0 86.82 0 11.07 2.11 0 0 0 0 2 12 0 0 0 0 0 11.072.11 0 0 0 86.82 2 13 0 0 0 0 0 11.07 2.11 0 0 86.82 0 2 14 0 86.82 0 00 11.07 2.11 0 0 0 0 2 15 0 0 0 0 0 11.07 2.11 0 0 0 0 2 16 0 0 0 0 0 00 0 0 0 0 3 1 0 0 0 46.6 0 6.79 0 0 0 0 0 3 2 0 0 0 0 0 6.79 0 0 0 046.6 3 3 0 0 0 0 0 6.79 0 0 0 46.6 0 3 4 0 46.6 0 0 0 6.79 0 0 0 0 0 3 50 6 0 0 0 6.79 0 0 0 0 0 3 6 0 0 0 84.2 0 12.27 0 3.54 0 0 0 3 7 0 0 0 00 12.27 0 3.54 0 0 84.2 3 8 0 0 0 0 0 12.27 0 3.54 0 84.2 0 3 9 0 84.2 00 0 12.27 0 3.54 0 0 0 3 10 0 0 0 0 0 12.27 0 3.54 0 0 0 3 11 0 0 084.22 0 12.27 3.51 0 0 0 0 3 12 0 0 0 0 0 12.27 3.51 0 0 0 84.22 3 13 00 0 0 0 12.27 3.51 0 0 84.22 0 3 14 0 34.22 0 0 0 12.27 3.51 0 0 0 0 315 0 0 0 0 0 12.27 3.51 0 0 0 0 3 16 0 0 0 0 0 0 0 0 0 0 0 4 1 0 0 046.08 0 7.83 0 0 0 0 0 4 2 0 0 0 0 0 7.83 0 0 0 0 46.08 4 3 0 0 0 0 07.83 0 0 0 46.08 0 4 4 0 46.08 0 0 0 7.83 0 0 0 0 0 4 5 0 0 0 0 0 7.83 00 0 0 0 4 6 0 0 0 80.95 0 13.76 0 5.29 0 0 0 4 7 0 0 0 0 0 13.76 0 5.290 0 80.95 4 8 0 0 0 0 0 13.76 0 5.29 0 80.95 0 4 9 0 50.95 0 0 0 13.76 05.29 0 0 0 4 10 0 0 0 0 0 13.76 0 5.29 0 0 0 4 11 0 0 0 80.98 0 13.775.25 0 0 0 0 4 12 0 0 0 0 0 13.77 5.25 0 0 0 80.98 4 13 0 0 0 0 0 13.775.25 0 0 80.98 0 4 14 0 30.98 0 0 0 13.77 5.25 0 0 0 0 4 15 0 0 0 0 013.77 5.25 0 0 0 0 4 16 0 0 0 0 0 100 0 0 0 0 0 5 1 0 0 0 45.37 0 9.26 00 0 0 0 5 2 0 0 0 0 0 9.26 0 0 0 0 45.37 5 3 0 0 0 0 0 9.26 0 0 0 45.370 5 4 0 45.37 0 0 0 9.26 0 0 0 0 0 5 5 0 0 0 0 0 9.26 0 0 0 0 0 5 6 0 00 76.8 0 15.67 0 7.53 0 0 0 5 7 0 0 0 0 0 15.67 0 7.53 0 0 76.8 5 8 0 00 0 0 15.67 0 7.53 0 76.8 0 5 9 0 76.8 0 0 0 15.67 0 7.53 0 0 0 5 10 0 00 0 0 15.67 0 7.53 0 0 0 5 11 0 0 0 76.85 0 15.68 7.47 0 0 0 0 5 12 0 00 0 0 15.68 7.47 0 0 0 76.85 5 13 0 0 0 0 0 15.68 7.47 0 0 76.85 0 5 140 76.85 0 0 0 15.68 7.47 0 0 0 0 5 15 0 0 0 0 0 15.68 7.47 0 0 0 0 5 160 0 0 0 0 0 0 0 0 0 0 6 1 0 0 0 44.35 0 11.31 0 0 0 0 0 6 2 0 0 0 0 011.31 0 0 0 0 44,35 6 3 0 0 0 0 0 11.31 0 0 0 44.35 0 6 4 0 44.35 0 0 011.31 0 0 0 0 0 6 5 0 0 0 0 0 11.31 0 0 0 0 0 6 6 0 0 0 71.33 0 18.19 010.49 0 0 0 6 7 0 0 0 0 0 18.19 0 10.49 0 0 71.33 6 8 0 0 0 0 0 18.19 010.49 0 71.33 0 6 9 0 71.33 0 0 0 18.19 0 10.49 0 0 0 6 10 0 0 0 0 018.19 0 10.49 0 0 0 6 11 0 0 0 71.39 0 18.2 10.41 0 0 0 0 6 12 0 0 0 0 018.2 10.41 0 10 0 /1.39 6 13 0 0 0 0 0 18.2 10.41 0 0 71.39 0 6 14 071.39 0 0 0 18.2 10.41 0 0 0 0 6 15 0 0 0 0 0 18.2 10.41 0 0 0 0 6 16 00 0 0 0 0 0 0 0 0 0 7 1 0 0 0 42.74 0 14.53 0 0 0 Q 0 7 2 0 0 0 0 014.53 0 0 0 0 42.74 7 3 0 0 0 0 0 14.53 0 0 0 42.74 0 7 4 0 42.74 0 0 014.53 0 0 0 0 0 7 5 0 0 0 0 0 14.53 0 0 0 0 0 7 6 0 0 0 63.75 0 21.67 014.58 0 0 0 7 7 0 0 0 0 0 21.67 0 14.58 0 0 63.75 7 8 0 0 0 0 0 21.67 014.58 0 63.75 0 7 9 0 63.75 0 0 0 21.67 0 14.58 0 0 0 7 10 0 0 0 0 021.67 0 14.58 0 0 0 7 11 0 0 0 63.82 0 21.7 14.48 0 0 0 0 7 12 0 0 0 0 021.7 14.48 0 0 0 63.82 7 13 0 0 0 0 0 21.7 14.48 0 0 63.82 0 7 14 063.82 0 0 0 21.7 14.48 0 0 0 0 7 15 0 0 0 0 0 21.7 14.48 0 0 0 0 7 16 00 0 0 0 100 0 0 0 0 0 8 1 0 0 0 39.84 0 20.32 0 0 0 0 0 8 2 0 0 0 0 020.32 0 0 0 0 39.84 8 3 0 0 0 0 0 20.32 0 0 0 39.84 0 8 4 0 39.84 0 0 020.32 0 0 0 0 0 8 5 0 0 0 0 0 20.32 0 0 0 0 0 8 6 0 0 0 52.58 0 26.81 020.61 0 0 0 8 7 0 0 0 0 0 26.81 0 20.61 0 0 52.58 8 8 0 0 0 0 0 26.81 020.61 0 52.58 0 8 9 0 52.58 0 0 0 26.81 0 20.61 0 0 0 8 10 0 0 0 0 026.81 0 20.61 0 0 0 8 11 0 0 0 52.66 0 26.86 20.48 0 0 0 0 8 12 0 0 0 00 26.86 20.48 0 0 0 52.66 8 13 0 0 0 0 0 26.86 20.48 0 0 52.66 0 8 14 052.66 0 0 0 26.86 20.48 0 0 0 0 8 15 0 0 0 0 0 26.86 20.48 0 0 0 0 8 160 0 0 0 0 0 0 0 0 0 0 9 1 34.63 0 0 0 0 22.08 0 0 0 0 0 9 2 0 0 0 0 016.67 0 0 26.14 0 0 9 3 0 0 0 0 21 13.39 0 0 0 0 0 9 4 0 0 51.55 0 06.57 0 0 0 0 0 9 5 0 0 0 0 0 5.99 0 0 0 0 0 9 6 56.82 0 0 0 0 36.22 06.96 0 0 0 9 7 0 0 0 0 0 36.22 0 6.96 56.82 0 0 9 8 0 0 0 0 56.82 36.220 6.96 0 0 0 9 9 0 0 86.81 0 0 11.07 0 2,13 0 0 0 9 10 0 0 0 0 0 11.07 02.13 0 0 0 9 11 56.85 0 0 0 0 36.24 6.91 0 0 0 0 9 12 0 0 0 0 0 36.246.91 0 56.85 0 0 9 13 0 0 0 0 56.85 36.24 6.91 0 0 0 0 9 14 0 0 86.82 00 11.07 2.11 0 0 0 0 9 15 0 0 0 0 0 11.07 2.11 0 0 0 0 9 16 0 0 0 0 0 00 0 0 0 0 10 1 32.11 0 0 0 0 22.93 0 0 0 0 0 10 2 0 0 0 0 0 17.15 0 024.01536998 0 0 10 3 0 0 0 0 19.18 13.69 0 0 0 0 0 10 4 0 0 48.71 0 06.96 0 0 0 0 0 10 5 0 0 0 0 0 6.31 0 0 0 0 0 10 6 52.36 0 0 0 0 37.38 010.26 0 0 0 10 7 0 0 0 0 0 37.38 0 10.26 52.36 0 0 10 8 0 0 0 0 52.3637.38 0 10.26 0 0 0 10 9 0 0 84.6 0 0 12.08 0 3.32 0 0 0 10 10 0 0 0 0 012.08 0 3.32 0 0 0 10 11 52.4 0 0 0 0 37.41 10.19 0 0 0 0 10 12 0 0 0 00 37.41 10.19 0 52.4 0 0 10 13 0 0 0 0 52.4 37.41 10.19 0 0 0 0 10 14 00 84.63 0 0 12.08 3.29 0 0 0 0 10 15 0 0 0 0 0 12.08 3.29 0 0 0 0 10 160 0 0 0 0 100 0 0 0 0 0 11 1 29.39 0 0 0 0 23.85 0 0 0 0 0 11 2 0 0 0 00 17.66 0 0 21.76 0 0 11 3 0 0 0 0 17.28 14.02 0 0 0 0 0 11 4 0 0 45.530 0 7.39 0 0 0 0 0 11 5 0 0 0 0 0 6.66 0 0 0 0 0 11 6 47.6 0 0 0 0 38.620 13.78 0 0 0 11 7 0 0 0 0 0 38.62 0 13.78 47.6 0 0 11 8 0 0 0 0 47.638.62 0 13.78 0 0 0 11 9 0 0 81.95 0 0 13.3 0 4.75 0 0 0 11 10 0 0 0 0 013.3 0 4.75 0 0 0 11 11 47.65 0 0 0 0 38.66 13.68 0 0 0 0 11 12 0 0 0 00 38.66 13.68 0 47.65 0 0 11 13 0 0 0 0 47.65 38.66 13.68 0 0 0 0 11 140 0 81.99 0 0 13.3 4.71 0 0 0 0 11 15 0 0 0 0 0 13.3 4.71 0 0 0 0 11 160 0 0 0 0 0 0 0 0 0 0 12 1 26.44 0 0 0 0 24.84 0 0 0 0 0 12 2 0 0 0 0 018.2 0 0 19.37 0 0 12 3 0 0 0 0 15.28 14.35 0 0 0 0 0 12 4 0 0 41.92 0 07.88 0 0 0 0 0 12 5 0 0 0 0 0 7.06 0 0 0 0 0 12 6 42.52 0 0 0 0 39.94 017.54 0 0 0 12 7 0 0 0 0 0 39.94 0 17.54 42.52 0 0 12 8 0 0 0 0 42.5239.94 0 17.54 0 0 0 12 9 0 0 78.71 0 0 14.79 0 6.5 0 0 0 12 10 0 0 0 0 014.79 0 6.5 0 0 0 12 11 42.58 0 0 0 0 40 17.42 0 0 0 0 12 12 0 0 0 0 040 17.42 0 42.58 0 0 12 13 0 0 0 0 42.58 40 17.42 0 0 0 0 12 14 0 078.76 0 0 14.8 6.45 0 0 0 0 12 15 0 0 0 0 0 14.8 6.45 0 0 0 0 12 16 0 00 0 0 0 0 0 0 0 0 13 1 23.24 0 0 0 0 25.93 0 0 0 0 0 13 2 0 0 0 0 018.77 0 0 16.82 0 0 13 3 0 0 0 0 13.19 14.71 0 0 0 0 0 13 4 0 0 37.81 00 8.44 0 0 0 0 0 13 5 0 0 0 0 0 7.5 0 0 0 0 0 13 6 37.07 0 0 0 0 41.36 021.57 0 0 0 13 7 0 0 0 0 0 41.36 0 21.57 37.07 0 0 13 8 0 0 0 0 37.0741.36 0 21.57 0 0 0 13 9 0 0 74.65 0 0 16.66 0 8.69 0, 0 0 13 10 0 0 0 00 16.66 0 8.69 0 0 0 13 11 37.14 0 0 0 0 41.43 21.43 0 0 0 0 13 12 0 0 00 0 41.43 21.43 0 37.14 0 0 13 13 0 0 0 0 37.14 41.43 21.43 0 0 0 0 1314 0 0 74.71 0 0 16.67 8.62 0 0 0 0 13 15 0 0 0 0 0 16.67 8.62 0 0 0 013 16 0 0 0 0 0 100 0 0 0 0 0 14 1 19.74 0 0 0 0 27.11 0 0 0 0 0 14 2 00 0 0 0 19.38 0 0 14.12 0 0 14 3 0 0 0 0 10.98 15.08 0 0 0 0 0 14 4 0 033.06 0 0 9.08 0 0 0 0 0 14 5 0 0 0 0 0 8.01 0 0 0 0 0 14 6 31.23 0 0 00 42.88 0 25.89 0 0 0 14 7 0 0 0 0 0 42.88 0 25.89 31.23 0 0 14 8 0 0 00 31.23 42.88 0 25.89 0 0 0 14 9 0 0 69.42 0 0 19.06 0 11.51 0 0 0 14 100 0 0 0 0 19.06 0 11.51 0 0 0 14 11 31.29 0 0 0 0 42.97 25.74 0 0 0 0 1412 0 0 0 0 0 42.97 25.74 0 31.29 0 0 14 13 0 0 0 0 31.29 42.97 25.74 0 00 0 14 14 0 0 69.49 0 0 19.08 11.43 0 0 0 0 14 15 0 0 0 0 0 19.08 11.430 0 0 0 14 16 0 0 0 0 0 0 0 0 0 0 0 15 1 15.91 0 0 0 0 28.4 0 0 0 0 0 152 0 0 0 0 0 20.03 0 0 11.22 0 0 15 3 0 0 0 0 8.67 15.47 0 0 0 0 0 15 4 00 27.53 0 0 9.83 0 0 0 0 0 15 5 0 0 0 0 0 8.59 0 0 0 0 0 15 6 24.94 0 00 0 44.51 0 30.55 0 0 0 15 7 0 0 0 0 0 44.51 0 30.55 24.94 0 0 15 8 0 00 0 24.94 44.51 0 30.55 0 0 0 15 9 0 0 62.42 0 0 22.28 0 15.29 0 0 0 1510 0 0 0 0 0 22.28 0 15.29 0 0 0 15 11 25 0 0 0 0 44.63 30.37 0 0 0 0 1512 0 0 0 0 0 44.63 30.37 0 25 0 0 15 13 0 0 0 0 25 44.63 30.37 0 0 0 015 14 0 0 62.5 0 0 22.31 15.19 0 0 0 0 15 15 0 0 0 0 0 22.31 15.19 0 0 00 15 16 0 0 0 0 0 0 0 0 0 0 0 16 1 11.7 0 0 0 0 29.82 0 0 0 0 0 16 2 0 00 0 0 20.73 0 0 8.13 0 0 16 3 0 0 0 0 6.23 15.89 0 0 0 0 0 16 4 0 021.01 0 0 10.71 0 0 0 0 0 16 5 0 0 0 0 0 9.26 0 0 0 0 0 16 6 18.15 0 0 00 46.28 0 35.57 0 0 0 16 7 0 0 0 0 0 46.28 0 35.57 18.15 0 0 16 8 0 0 00 18.15 46.28 0 35.57 0 0 0 16 9 0 0 52.58 0 0 26.81 0 20.61 0 0 0 16 100 0 0 0 0 26.81 0 20.61 0 0 0 16 11 18.2 0 0 0 0 46.41 35.38 0 0 0 0 1612 0 0 0 0 0 46.41 35.38 0 18.2 0 0 16 13 0 0 0 0 18.2 46.41 35.38 0 0 00 16 14 0 0 52.66 0 0 26.86 20.48 0 0 0 0 16 15 0 0 0 0 0 26.86 20.48 00 0 0 16 16 0 0 0 0 0 100 0 0 0 0 0

[0299] TABLE V Tem- pera- ture: 250 C. Pt1.O%/ R C COCONV H2OCONVCO2PROD CO2PERPROD CH4PROD Zr02_std CeNO33 NH42CeNO36 CONO32 CoOAC2Na3CoNO36 real real real real real real real real real real real realreal 1 1 29.8402 21.1977 1.0839 39.7897 0.1693 0.1275 0 0 0 0 0 1 2−0.8066 −0.3468 0.0199 0.7318 0.015 0 0 0 0 0 0 1 3 −1.342 −0.8883−0.0103 −0.3788 0.0069 0 0 0 0 0 0 1 4 −0.4471 −0.8737 −0.0209 −0.76790.0045 0 0 0 0 0 0 1 5 0.2051 −0.7078 0.0201 0.7386 0.0086 0 0 0 0 0 0 16 −0.2701 −1.1286 0.0074 −0.273 0.0008 0 0 0 0 0 0 1 7 28.4296 17.03960.9422 34.5858 0.1303 0.1275 0 0 0 0 0 1 8 0.3481 −0.0616 −0.0199−0.7298 −0.0025 0 0 0 0 0 0 1 9 −0.1214 −1.3018 −0.0217 −0.7951 1.001 00 0 0 0 0 1 10 1.2904 −0.1752 −0.0251 −0.9203 −0.0045 0 0 0 0 0 0 1 11−0.1983 −0.4964 −0.0223 −0.8192 0.0005 0 0 0 0 0 0 1 12 −0.0741 −1.2392−0.019 −0.6989 0.0004 0 0 0 0 0 0 1 13 27.9999 15.9352 0.9526 34.96870.128 0.1275 0 0 0 0 0 1 14 0.6232 −0.3023 0.0112 0.4122 0.0003 0 0 0 00 0 1 15 −0.1018 0.0336 0.0235 −0.8632 −0.0047 0 0 0 0 0 0 1 16 27.235116.5803 0.888 32.5966 0.1185 0.1275 0 0 0 0 0 2 1 25.6429 17.9695 0.831330.5152 0.0986 0 0 0 0.125 0 0 2 2 29.4104 18.6834 0.9576 35.1519 0.11860 0 0.5 0.125 0 0 2 3 22.3392 8.9723 0.6239 22.9019 0.1378 0 0 0 0.125 00 2 4 0.8395 0.2708 0.0014 0.0528 0.0013 0 0 0 0.125 0 0 2 5 22.452513.4385 0.672 24.6699 0.1033 0 0 0 0.125 0.5 0 2 6 30.6495 18.9614 1.02837.7387 0.136 0 0 0 0.125 0 0.5 2 7 22.8992 14.6855 0.7054 25.89490.0994 0 0 0 0.125 0 0 2 8 16.4705 11.3025 0.4957 18.197 0.0643 0 0 00.125 0 0 2 9 25.2898 17.1191 0.8418 30.903 0 0 0 0 0.125 0 0 2 1027.7651 17.855 0.9307 34.1645 0.1134 0 0.5 0 0.125 0 0 2 11 15.235310.1525 0.5062 18.5825 0.0625 0 0 0 0.125 0 0 2 12 6.6516 1.7768 0.20277.4414 0.0231 0 0 0 0.125 0 0 2 13 5.6662 4.3865 0.1536 5.6377 0.0183 00 0 0.125 0 0 2 14 20.5443 12.549 0.6838 25.1023 0.0868 0 0 0 0.125 0 02 15 2.2164 0.1212 0.0573 2.1049 0.0061 0 0 0 0 0 0 2 16 0.393 1.30110.0224 0.821 0.0062 0 0 0 0 0 0 3 1 22.2454 15.3754 0.7105 26.08260.0816 0 0 0 0.2188 0 0 3 2 28.0083 19.5547 0.885 32.4878 0.1083 0 00.4063 0.2188 0 0 3 3 23.6895 14.2896 0.6787 24.9136 0.1246 0 0 0 0.21880 0 3 4 0.9693 2.2659 0.0302 1.1081 0.0146 0 0 0 0.2188 0 0 3 5 28.274216.4476 0.8881 32.6016 0.1315 0 0 0 0.2188 0.4063 0 3 6 40.4567 21.97040.2225 44.8759 0.2055 0 0 0 0.2188 0 0.4063 3 7 25.2346 17.7275 0.807929.6585 0.1051 0 0 0 0.2188 0 0 3 8 23.7508 16.0999 0.736 27.0183 0.10410 0 0 0.2188 0 0 3 9 26.3184 9.4909 0.8642 31.7233 0.098 0 0 0 0.2188 00 3 10 26.3066 7.5553 0.8712 31.9817 0.1009 0 0.4063 0 0.2188 0 0 3 116.5069 2.0298 0.525 9.2728 0.0577 0 0 0 0.2188 0 0 3 12 15.7501 1.82250.4936 8.1205 0.0521 0 0 0 0.2188 0 0 3 13 6.2855 5.3787 0.1728 6.34320.01 0 0 0 0.2188 0 0 3 14 18.4215 4.2445 0.619 22.7235 0.0672 0 0 00.2188 0 0 3 15 1.6097 3.5749 0.0233 0.8544 0.0089 0 0 0 0.2188 00 0 316 1.3509 0.7363 0.0005 0.0168 0.0077 0 0 0 0 0 0 4 1 23.1744 6.98660.7784 28.5757 0.0904 0 0 0 0.3125 0 0 4 2 28.5323 20.2685 0.916133.6276 0.112 0 00 0.3125 0.3125 00 0 4 3 24.9023 6.5852 0.7687 28.21990.1184 0 0 0 0.3125 0 0 4 4 8.3484 7.4139 0.2462 9.0365 0.0236 0 0 00.3125 0 0 4 5 28.2314 6.652 0.814 29.8824 0.1533 0 0 0 0.3125 0.3125 04 6 39.4798 24.09 1.1719 3.0211 0.2026 0 0 0 0.3125 0 0.3125 4 7 25.06577.1429 0.7976 29.2776 0.105 0 0 0 0.3125 0 0 4 8 20.8684 14.4244 0.648423.8022 0.0887 0 0 0 0.3125 0 5 4 9 26.476 18.4214 0.8784 32.2449 0.10050 0 0 0.3125 0 0 4 10 25.3804 18.1039 0.8522 31.2829 3.0975 0 0.3125 00.3125 0 0 4 11 13.9181 9.2274 3.4588 16.8412 0.0498 0 0 0 0.3125 0 0 412 13.6987 10.4619 0.434 15.9319 0.0459 0 0 0 0.3125 0 0 4 13 8.0697.5589 0.2327 8.5431 0.0185 0 0 0 0.3125 0 0 4 14 21.7048 15.5036 0.723726.5651 0.0794 0 0 0 0.3125 0 0 4 15 7.1383 7.611 0.2204 8.0914 0.0168 00 0 0.3125 0 0 4 16 28.2274 18.5972 0.9383 34.4443 0.1182 0.1275 0 0 0 00 5 1 25.0356 17.8739 0.8182 30.0351 0.0996 0 0 0 0.4063 0 0 5 2 29.521121.5832 3.9284 34.0807 0.1135 0 0 0.2188 0.4063 0 0 5 3 25.5889 17.36110.7957 29.211 0.1149 0 0 0 0.4063 0 0 5 4 11.1187 9.9822 0.3389 12.44170.0338 0 0 0 3.4063 0 0 5 5 27.9457 16.713 0.8317 30.5293 0.1491 0 0 00.4063 0.2188 0 5 6 38.1172 21.2674 1.1043 40.539 0.2047 0 0 0 0.4063 00.2188 5 7 24.6847 17.5415 0.8004 29.3828 0.098 0 0 0 0.4063 0 0 5 824.8369 17.0456 0.7916 29.0571 0.1039 0 0 0 0.4063 0 0 5 9 25.268419.1268 0.8271 30.3624 0.0942 0 0 0 0.4063 0 0 5 10 25.9949 19.50890.8585 31.5149 0.0991 0 0.2188 0 0.4063 0 0 5 11 17.6559 13.8567 0.577521.1997 0.0635 0 0 0 0.4063 0 0 5 12 19.56 14.366 0.6131 22.5058 0.07050 0 0 0.4063 0 0 5 13 7.807 6.7271 0.2181 8.005 0.021 0 0 0 0.4063 0 0 514 22.2026 14.967 0.748 27.4571 5.0898 0 0 0 0.4063 0 0 5 15 11.41618.8494 0.3588 13.173 0.0373 0 0 0 0.4063 0 0 5 16 0.0343 0.2746 −0.0017−0.0622 −0.007 0 0 0 0 0 0 6 1 28.3635 19.4266 0.9197 33.7623 0.1222 0 00 0.5 0 0 6 2 30.4663 20.8458 0.9865 36.2151 0.1288 0 0 0.125 0.5 0 0 63 24.5123 16.1173 0.794 29.1455 0.1075 0 0 0 0.5 0 0 6 4 20.2767 14.69180.6733 24.7161 0.0801 0 0 0 0.5 0 0 6 5 33.2496 16.76 0.9351 34.32740.2217 0 0 0 3.5 0.125 0 6 6 38.5058 19.2941 1.0938 40.154 0.2327 0 0 00.5 5 0.125 6 7 24.1336 17.4112 0.7994 29.3455 5.1052 0 0 0 0.5 0 0 6 822.6528 14.9365 0.7653 28.0945 0.0974 0 0 0 0.5 0 0 6 9 26.9144 19.68020.8845 32.4702 0.1055 0 0 0 0.5 0 0 6 10 26.6038 18.7414 0.9208 33.80010.11 0 0.125 0 0.5 0 0 6 11 22.4349 14.9258 0.7817 28.6959 0.0944 0 0 00.5 0 0 6 12 20.9112 14.2122 0.6922 25.4099 0.0817 0 0 0 0.5 0 0 6 1311.904 7.5826 0.4014 14.7338 0.0486 0 0 0 0.5 0 0 6 14 23.5252 16.73110.7707 28.2915 0.0917 0 0 0 0.5 0 0 6 15 17.2103 10.833 0.5735 21.05130.067 0 0 0 0.5 0 0 6 16 1.0088 −0.1805 0.0177 0.6503 −0.0041 0 0 0 0 00 7 1 29.1091 18.3888 0.9377 34.4238 0.1288 0 0 0 0 0 0 7 2 23.467515.9929 0.7993 29.3427 0.1033 0 0 0 0.5 0 0 7 3 24.4 17.9806 0.805229.5583 0.0931 0 0 0.5 0 0 0 7 4 23.9259 17.6284 0.8206 30.1251 0.0928 00 0 0 0 0 7 5 21.9374 15.2657 0.7495 27.5124 0.0915 0 0 0 0 0.5 0 7 634.6888 23.3528 1.131 41.5182 0.1544 0 0 0 0 0 0 7 7 23.0341 16.94950.7009 25.7276 0.099 0 0 0 0 0 0 7 8 28.7153 15.6433 0.8015 29.42210.1671 0 0 0 0 0 0 7 9 21.8886 15.6142 0.7632 28.0152 0.0898 0 0 0 0 0 07 10 21.9107 15.6183 0.7745 28.4325 0.0907 0 0 0 0 0 0 7 11 18.590714.206 0.615 22.5768 0.0714 0 0 0 0 0 0 7 12 24.8013 17.9553 0.839130.8011 0.1049 0 0 0 0 0 0 7 13 4.148 4.5963 0.1558 5.7193 0.01 0 0 0 00 0 7 14 25.1707 16.9965 0.8683 31.875 0.1033 0 0 0 0 0 0 7 15 0.0537.9852 0.3638 13.3549 0.0383 0 0 0 0 0 0 7 16 27.3338 18.6129 0.931434.1925 0.1154 0.1275 0 0 0 0 0 8 1 27.8709 16.8374 0.9039 33.17990.1419 0 0 0 0 0 0 8 2 25.0239 16.3557 0.8605 31.5885 0.1186 0 0 00.4063 0 0 8 3 23.3124 16.5445 0.7803 28.6442 0.1016 0 0 0.4063 0 0 0 84 30.4167 20.755 1.0121 37.1518 0.1278 0 0 0 0 0 0 8 5 22.4729 15.59520.7556 27.7364 0.0987 0 0 0 0 0 0 8 6 33.8859 22.7736 1.1246 41.28290.1534 0 0 0 0 0 0.4063 8 7 23.0982 15.007 0.72 26.4315 0.1098 0 0 0 0 00 8 8 27.9822 13.7786 0.811 29.7729 0.1778 0 0 0 0 0 0 8 9 23.730517.1175 0.8213 30.1477 0.1059 0 0 0 0 0 0 8 10 24.1435 16.057 0.805829.5803 0.1029 0 0.4063 0 0 0 0 8 11 22.7845 15.9341 0.7662 28.1260.1051 0 0 0 0 0 0 8 12 22.5472 14.8209 0.7762 28.4929 0.1038 0 0 0 0 00 8 13 4.6 5.0283 0.1611 5.9139 0.0164 0 0 0 0 0 0 8 14 26.3117 17.55680.8937 32.8057 0.1158 0 0 0 0 0 0 8 15 19.2935 13.6483 0.7008 25.7250.0827 0 0 0 0 0 0 8 16 0.3501 2.3807 0.0044 0.1601 −0.0072 0 0 0 0 0 09 1 30.2669 17.4031 0.9382 34.439 0.1638 0 0 0 0 0 0 9 2 24.7831 15.51680.8133 29.856 0.1193 0 0 0 0.3125 0 0 9 3 24.8843 16.3799 0.8144 29.89520.1144 0 0 0.3125 0 0 0 9 4 27.7158 18.3043 0.9486 34.8222 0.1209 0 0 00 0 0 9 5 22.301 14.7031 0.7678 28.1862 3.1077 0 0 0 0 0.3125 0 9 631.7529 21.8186 1.0511 38.5834 0.1407 0 0 0 0 0 0.3125 9 7 22.422313.2509 0.6914 25.3794 0.1125 0 0 0 0 0 0 9 8 26.7272 10.823 0.796629.2411 0.1718 0 0 0 0 0 0 9 9 18.6358 11.9972 0.6423 23.5776 0.0893 0 00 0 0 0 9 10 21.5732 13.0857 0.7295 26.7785 0.0998 0 0.3125 0 0 0 0 9 1121.8603 13.7562 0.7383 27.1031 0.1087 0 0 0 0 0 0 9 12 23.2584 14.23390.7779 28.5546 0.1092 0 0 0 0 0 0 9 13 6.1089 5.8813 0.2145 7.87370.0226 0 0 0 0 0 0 9 14 21.796 14.0238 0.7518 27.5966 0.1012 0 0 0 0 0 09 15 14.7758 10.7605 0.524 19.2341 0.0608 0 0 0 0 0 0 9 16 0.0047 0.36210.0345 1.268 0.0006 0 0 0 0 0 0 10 1 32.2957 12.969 0.8786 32.253 0.22590 0 0 0 0 0 10 2 22.9073 13.5906 0.7444 27.3268 0.1229 0 0 0 0.2188 0 010 3 24.02 14.4655 0.7658 28.1101 0.1285 0 0 0.2188 0 0 0 10 4 27.473518.2379 0.9287 34.0901 0.1247 0 0 0 0 0 0 10 5 25.7888 14.3222 0.790829.0301 0.1508 0 0 0 0 0.2188 0 10 6 28.2681 18.4984 0.959 35.20410.1403 0 0 0 0 0 0.2188 10 7 26.3335 13.7746 0.7698 28.257 0.1587 0 0 00 0 0 10 8 27.2793 11.6159 0.7715 28.3222 0.181 0 0 0 0 0 0 10 9 23.753213.9992 0.7647 28.0727 0.1187 0 0 0 0 0 0 10 10 23.0104 12.8612 0.750127.5368 0.1242 0 0.2188 0 0 0 0 10 11 24.3958 13.8516 0.7821 28.70850.1283 0 0 0 0 0 0 10 12 24.7178 14.4298 0.7945 29.1648 0.1251 0 0 0 0 00 10 13 6.2103 5.4757 0.2329 8.5508 0.0276 0 0 0 0 0 0 10 14 20.325913.0573 0.6932 25.4467 0.0987 0 0 0 0 0 0 10 15 18.1743 12.8071 0.668524.5392 0.0818 0 0 0 0 0 0 10 16 25.148 16.3311 0.9105 33.4226 0.11590.1275 0 0 0 0 0 11 1 33.2657 13.7869 0.9096 33.389 0.2236 0 0 0 0 0 011 2 26.3629 12.996 0.8123 29.819 0.1618 0 0 0 0.125 0 0 11 3 24.966113.9343 0.8015 29.4223 0.135 0 0 0.125 0 0 0 11 4 25.749 14.2206 0.856231.4286 0.1402 0 0 0 0 0 0 11 5 23.3622 11.0514 0.726 26.6504 0.1408 0 00 0 0.125 0 11 6 25.4002 15.3152 0.8622 31.652 0.1297 0 0 0 0 0 0.125 117 23.7527 11.0405 0.7081 25.9945 0.1474 0 0 0 0 0 0 11 8 25.2713 10.45180.7606 27.9193 0.1663 0 0 0 0 0 0 11 9 22.1004 12.2049 0.7055 25.89810.1177 0 0 0 0 0 0 11 10 21.8975 12.2273 0.7148 26.2406 0.1184 0 0.125 00 0 0 11 11 22.2123 12.4559 0.7208 26.4587 0.1235 0 0 0 0 0 0 11 1222.4272 13.3655 0.7375 27.0716 0.1141 0 0 0 0 0 0 11 13 10.6819 7.06260.3567 13.095 0.0525 0 0 0 0 0 0 11 14 22.4528 12.9362 0.7568 27.78010.1206 0 0 0 0 0 0 11 15 9.7448 13.9333 0.6951 25.5175 0.0875 0 0 0 0 00 11 16 0.1972 1.471 0.0237 0.8717 0.0002 0 0 0 0 0 0 12 1 31.565621.6797 1.0782 39.5788 0.1397 0 0 0 0 0 0 12 2 9.6043 3.572 0.695525.5322 0.089 0 0 0 0.5 0 0 12 3 28.1666 7.3647 0.9244 33.9334 0.1488 00 0 0 0 0 12 4 31.3253 21.7961 1.0594 38.89 0.1349 0 0 0.5 0 0 0 12 57.3834 14.0571 0.6238 22.8995 0.0749 0 0 0 0 0.5 0 12 6 35.3057 24.55211.1878 43.6046 0.1566 0 0 0 0 0 0.5 12 7 23.1431 16.6639 0.8015 29.42110.1066 0 0 0 0 0 0 12 8 26.6065 17.7981 0.9318 34.2045 0.1338 0 0 0 0 00 12 9 31.073 22.4346 1.0697 39.269 0.1354 0 0 0 0 0 0 12 10 29.932822.2939 1.0514 38.5962 0.1273 0 0.5 0 0 0 0 12 11 28.5736 20.9007 1.012537.1693 0.1236 0 0 0 0 0 0 12 12 28.8195 9.4676 1.0399 38.1729 0.1274 00 0 0 0 0 12 13 2.9218 3.3576 0.0985 3.6155 0.0097 0 0 0 0 0 0 12 1425.7013 7.9671 0.9023 33.1211 0.1147 0 0 0 0 0 0 12 15 8.492 5.91260.3308 12.1433 0.0423 0 0 0 0 0 0 12 16 −0.1015 0.1618 0.0165 0.60660.0023 0 0 0 0 0 0 13 1 32.929 23.1662 1.1398 41.8401 0.1451 0 0 0 0 0 013 2 12.9188 10.5882 0.449 16.481 0.0547 0 0 0 0.4063 0 0 13 3 28.085618.7043 0.9401 34.5103 0.126 0 0 0 0 0 0 13 4 31.7131 22.9009 1:05438.6919 0.1335 0 0 0.4063 0 0 0 13 5 10.3872 8.6629 0.3924 14.405 0.04540 0 0 0 0.4063 0 13 6 32.6469 22.0266 1.0976 40.2904 0.1422 0 0 0 0 00.4063 13 7 26.7979 19.1216 0.9313 34.1868 0.1168 0 0 0 0 0 0 13 827.1205 19.4829 0.9549 35.0517 0.1223 0 0 0 0 0 0 13 9 29.5931 21.52311.038 38.1041 0.1264 0 0 0 0 0 0 13 10 28.868 20.7843 1.0163 37.30680.1254 0 0.4063 0 0 0 0 13 11 19.8455 15.1061 0.6906 25.353 0.0865 0 0 00 0 0 13 12 28.8191 20.6337 1.0134 37.1994 0.1238 0 0 0 0 0 0 13 132.6024 3.2972 0.0961 3.526 0.0071 0 0 0 0 0 0 13 14 25.0501 16.21040.9126 33.5022 0.1159 0 0 0 0 0 0 13 15 6.4246 5.1337 0.2835 10.40710.0349 0 0 0 0 0 0 13 16 24.6043 16.341 0.9005 33.0556 0.1142 0.1275 0 00 0 0 14 1 31.1905 22.5852 1.0761 39.5045 0.1379 0 0 0 0 0 0 14 215.3686 12.5627 0.5534 20.3138 0.0672 0 0 0 0.3125 0 0 14 3 28.590221.079 0.9573 35.1415 0.1252 0 0 0 0 0 0 14 4 30.8225 21.6996 1.064839.0881 0.1372 0 0 0.3125 0 0 0 14 5 10.1619 9.3091 0.3843 14.10780.0446 0 0 0 0 0.3125 0 14 6 25.9037 19.3547 0.9378 34.425 0.1151 0 0 00 0 0.3125 14 7 28.9615 21.1086 0.9966 36.5847 0.129 0 0 0 0 0 0 14 825.3268 19.6253 0.9096 33.392 0.1117 0 0 0 0 0 0 14 9 30.5368 22.80981.0517 38.6072 0.1317 0 0 0 0 0 0 14 10 30.4639 21.8604 1.0468 38.42790.1319 0 0.3125 0 0 0 0 14 11 28.5368 20.5826 1.0152 37.2667 0.1262 0 00 0 0 0 14 12 28.9878 20.031 1.0283 37.748 0.1277 0 0 0 0 0 0 14 131.9405 3.4997 0.1021 3.7493 0.0083 0 0 0 0 0 0 14 14 26.2698 18.12590.9407 34.5326 0.1172 0 0 0 0 0 0 14 15 3.5222 3.4456 0.1728 6.3450.0193 0 0 0 0 0 0 14 16 1.2721 0.2876 0.0152 0.5574 0 0 0 0 0 0 0 15 121.9285 16.5533 0.7944 29.1616 0.0981 0 0 0 0 0 0 15 2 8.5556 7.93220.3176 11.6581 0.0386 0 0 0 0.2188 0 0 15 3 28.9139 19.3873 1.011537.1305 0.1329 0 0 0 0 0 0 15 4 29.4947 20.5675 1.0129 37.1816 0.1319 00 0.2188 0 0 0 15 5 10.3199 7.8183 0.3758 13.7939 0.0488 0 0 0 0 0.21880 15 6 19.07 12.9719 0.6822 25.0424 0.0872 0 0 0 0 0 0.2188 15 7 24.459216.5438 0.8787 32.2577 0.1122 0 0 0 0 0 0 15 8 26.1966 19.0364 0.928334.0753 0.1149 0 0 0 0 0 0 15 9 28.805 20.399 1.0007 36.7353 0.1231 0 00 0 0 0 15 10 27.8671 19.9279 0.9883 36.2797 0.1237 0 0.2188 0 0 0 0 1511 25.9077 18.1393 0.9238 33.9133 0.1174 0 0 0 0 0 0 15 12 26.816819.5131 0.9364 34.3739 0.1198 0 0 0 0 0 0 15 13 3.1831 4.1719 0.12554.6087 0.0135 0 0 0 0 0 0 15 14 25.6485 17.9831 0.9073 33.3061 0.1142 00 0 0 0 0 15 15 3.4019 2.8501 0.1862 6.8334 0.0252 0 0 0 0 0 0 15 16−0.6764 0.6935 0.0304 1.1161 0.0028 0 0 0 0 0 0 16 1 27.2358 17.97970.9948 36.5199 0.1324 0 0 0 0 0 0 16 2 20.4235 13.9408 0.7544 27.6930.0997 0 0 0 0.125 0 0 16 3 22.1148 16.7994 0.7919 29.0693 0.101 0 0 0 00 0 16 4 27.8457 8.1657 0.9706 35.6285 0.1316 0 0 0.125 0 0 0 16 516.0515 10.9271 0.6032 22.1443 0.0766 0 0 0 0 0.125 0 16 6 21.531916.4412 0.8048 29.5417 0.101 0 0 0 0 0 0.125 16 7 28.6538 19.2213 1.014537.243 0.1346 0 0 0 0 0 0 16 8 27.0582 20.0777 0.9481 34.8038 0.1218 0 00 0 0 0 16 9 28.251 19.2368 1.0097 37.0662 0.132 0 0 0 0 0 0 16 1028.3144 19.6597 0.9907 36.3661 0.1282 0 0.125 0 0 0 0 16 11 25.237217.9227 0.9037 33.1748 0.1146 0 0 0 0 0 0 16 12 27.1113 19.9798 0.98436.1202 0.1221 0 0 0 0 0 0 16 13 7.0222 6.86 0.2888 10.6009 0.0359 0 0 00 0 0 16 14 24.3113 16.5973 0.9032 33.1567 0.1156 0 0 0 0 0 0 16 1511.0117 7.8026 0.4408 16.1825 0.0553 0 0 0 0 0 0 16 16 24.9744 15.31360.9047 33.2092 0.1182 0.1275 0 0 0 0 0 Tem- pera- ture: 250 C. R CCuNO32 OeOX2 H2MOO4 KRuO4 RuNON033 RuNOOAc3 LaNO33 NH4ReO4 PtNH32NO22ZrONO32 ZrOOAc2 real real real real real real real real real real realreal real 1 1 0 0 0 0 0 0 0 0 0 0 0 1 2 0 0 0 0 0 0 0 0 0 0 0 1 3 0 0 00 0 0 0 0 0 0 0 1 4 0 0 0 0 0 0 0 0 0 0 0 1 5 0 0 0 0 0 0 0 0 0 0 0 1 60 0 0 0 0 0 0 0 0 0 0 1 7 0 0 0 0 0 0 0 0 0 0 0 1 8 0 0 0 0 0 0 0 0 0 00 1 9 0 0 0 0 0 0 0 0 0 0 1 1 10 0 0 0 0 0 0 0 0 0 0 0 1 11 0 0 0 0 0 00 0 0 0 0 1 12 0 0 0 0 0 0 0 0 0 0 0 1 13 0 0 0 0 0 0 0 0 0 1 0 1 14 0 00 0 0 0 0 0 0 0 0 1 15 0 0 0 0 0 0 0 0 0 1 0 1 16 0 0 0 0 0 0 0 0 0 0 02 1 0 0 0 0 0 0 0 0 0.1275 0 0 2 2 0 0 0 0 0 0 0 0 0.1275 0 0 2 3 0 0 00 0.0989 0 0 0 0.1275 0 0 2 4 0 0 0.5 0 0 0 0 0 0.1275 0 0 2 5 0 0 0 0 00 0 0 0.1275 0 0 2 6 0 0 0 0 0 0 0 0 0.1275 0 0 2 7 0 0 0 0.098 0 0 0 01.1275 0 0 2 8 0 0 0 0 0 0.098 0 0 0.1275 0 0 2 9 0 0 0 0 0 0 0.50 00.1275 0 0 2 10 0 0 0 0 0 0 0 0 0.1275 0 0 2 11 0 0 0 0 0 0 0 0 0.12751.5 0 2 12 0 0 0 0 0 0 0 0 0.1275 0 0.5 2 13 0.5 0 0 0 0 0 0 0 0.1275 10 2 14 0 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0 0.1275 0 0 13 5 0 0 0.2188 0 0 0 0 0 0.1275 0 0 13 6 0 0 0.2188 00 0 0 0 0.1275 0 0 13 7 0 0 0.2188 0.0796 0 0 0 0 0.1275 0 0 13 8 0 00.2188 0 0 0.0796 0 0 0.1275 0 0 13 9 0 0 0.2188 0 0 0 0.4063 0 0.1275 00 13 10 0 0 0.2188 0 0 0 0 0 0.1275 0 0 13 11 0 0 0.2188 0 0 0 0 00.1275 0.4063 0 13 12 0 0 0.2188 0 0 0 0 0 0.1275 0 0.4063 13 13 0.40630 0.2188 0 0 0 0 0 0.1275 0 0 13 14 0 0 0.2188 0 0 0 0 0.0873 0.1275 0 013 15 0 0.1625 0.2188 0 0 0 0 0 0.1275 0 0 13 16 0 0 0 0 0 0 0 0 0 0 014 1 0 0 0.3125 0 0 0 0 0 0.1275 0 0 14 2 0 0 0.3125 0 0 0 0 0 0.1275 00 14 3 0 0 0.3125 0 0.0618 0 0 0 0.1275 0 0 14 4 0 0 0.3125 0 0 0 0 00.1275 0 0 14 5 0 0 0.3125 0 0 0 0 0 0.1275 0 0 14 6 0 0 0.3125 0 0 0 00 0.1275 0 0 14 7 0 0 0.3125 0.0613 0 0 0 0 0.1275 0 0 14 8 0 0 0.3125 00 0.0613 0 0 0.1275 0 0 14 9 0 0 0.3125 0 0 0 0.3125 0 0.1275 0 0 14 100 0 0.3125 0 0 0 0 0 0.1275 0 0 14 11 0 0 0.3125 0 0 0 0 0 0.1275 0.31250 14 12 0 0 0.3125 0 0 0 0 0 0.1275 0 0.3125 14 13 0.3125 0 0.3125 0 0 00 0 0.1275 0 0 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0.0245 0 0 0.1275 0 0 16 9 0 0 0.5 0 0 00.125 0 0.1275 0 0 16 10 0 0 0.5 0 0 0 0 0 0.1275 0 0 16 11 0 0 0.5 0 00 0 0 0.1275 0.125 0 16 12 0 0 0.5 0 0 0 0 0 0.1275 0 0.125 16 13 0.1250 0.5 0 0 0 0 0 0.1275 0 0 16 14 0 0 0.5 0 0 0 0 0.0269 0.1275 0 0 16 150 0.05 0.5 0 0 0 0 0 0.1275 0 0 16 16 0 0 0 0 0 0 0 0 0 0 0 Temperature:250 C. SUM_(—) mol % mol % mol % mol % mol % mol % mol % mol % mol % mol% R C micromols Ce Co Cu Ge Mo Ru La Re Pt Zr real real 1 1 0.1275 0 0 00 0 0 0 0 100 0 1 2 0 0 0 0 0 0 0 0 0 0 0 1 3 0 0 0 0 0 0 0 0 0 0 0 1 41 0 0 0 0 0 0 0 0 0 0 1 5 0 0 0 0 0 0 0 0 0 0 0 1 6 0 0 0 0 0 0 0 0 0 00 1 7 0.1275 0 0 0 0 0 0 0 0 100 0 1 8 0 0 0 0 0 0 0 0 0 0 0 1 9 1 0 0 00 0 0 0 0 0 0 1 10 0 0 0 0 0 0 0 0 0 0 0 1 11 0 0 0 0 0 0 0 0 0 0 0 1 120 0 0 0 0 0 0 0 0 0 0 1 13 0.1275 0 0 0 0 0 0 0 0 100 0 1 14 0 0 0 0 0 01 0 0 0 0 1 15 0 0 0 0 0 0 0 0 0 0 0 1 16 0.1275 0 0 0 0 0 0 0 0 100 0 21 0.2525 0 49.5 0 0 0 0 0 0 50.5 0 2 2 0.7525 66.45 16.61 0 0 0 0 0 016.94 0 2 3 0.3514 0 35.57 0 0 0 28.14 0 0 36.28 0 2 4 1.7525 0 16.61 00 66.45 0 0 0 16.94 0 2 5 0.7525 0 83.06 0 0 0 0 0 0 16.94 0 2 6 0.75250 83.06 0 0 0 0 0 0 16.94 0 2 7 1.3505 0 35.66 0 0 0 27.96 0 0 36.38 0 28 0.3505 0 35.66 0 0 0 27.96 0 0 36.38 0 2 9 0.7525 0 16.61 0 0 0 066.45 0 16.94 0 2 10 0.7525 66.45 16.61 0 0 0 0 0 0 16.94 0 2 11 0.75250 16.61 0 0 0 0 0 1 16.94 66.45 2 12 0.7525 0 16.61 0 0 0 0 0 0 16.9466.45 2 13 0.7525 0 16.61 66.45 0 0 0 0 0 16.94 0 2 14 0.3599 0 34.73 00 0 0 0 29.84 35.43 0 2 15 0.4525 0 27.62 0 44.2 0 0 0 0 28.18 0 2 16 00 1 0 1 0 0 0 0 0 0 3 1 0.3463 0 63.18 0 0 0 0 0 0 36.82 0 3 2 0.752553.99 29.07 0 0 0 0 0 0 16.94 0 3 3 0.4266 0 51.28 0 0 0 18.84 0 0 29.890 3 4 0.7525 0 29.07 0 0 53.99 0 0 0 16.94 0 3 5 1.7525 0 83.06 0 0 0 00 0 16.94 0 3 6 0.7525 0 83.06 0 0 0 0 0 0 16.94 0 3 7 1.4259 0 51.36 00 1 18.7 0 0 29.94 0 3 8 0.4259 0 51.36 0 0 0 18.7 0 0 29.94 0 3 90.7525 0 29.07 0 0 0 0 53.99 0 16.94 0 3 10 0.7525 53.99 29.07 0 0 0 0 00 16.94 0 3 11 0.7525 0 29.07 0 0 0 0 0 0 16.94 53.99 3 12 0.7525 029.07 0 0 0 0 0 0 16.94 53.99 3 13 0.7525 0 29.07 53.99 0 0 0 0 0 16.940 3 14 1.4335 0 50.46 0 0 0 0 0 20.13 29.41 0 3 15 0.5088 0 43 0 31.94 00 0 0 25.06 0 3 16 0 0 0 0 0 0 0 0 0 0 0 4 1 0 0 71.02 0 0 0 0 0 0 28.980 4 2 0.7525 41.53 41.53 0 0 0 0 0 0 16.94 0 4 3 0.5018 0 62.27 0 0 012.32 0 0 25.41 0 4 4 0.7525 0 41.53 0 0 41.53 0 0 0 16.94 0 4 5 0.75251 83.06 0 1 1 0 0 0 16.94 0 4 6 0.7525 0 83.06 0 0 0 0 0 0 16.94 0 4 70.5013 0 62.34 0 0 0 12.22 0 0 25.44 0 4 8 0.5013 0 62.34 5 0 5 12.22 00 25.44 0 4 9 0.7525 0 41.53 0 0 0 0 41.53 0 16.94 0 4 10 0.7525 41.5341.53 0 0 0 0 0 0 16.94 0 4 11 0.7525 0 41.53 0 0 0 0 0 0 16.94 41.53 412 0.7525 0 41.53 0 0 5 0 0 5 16.94 41.53 4 13 0.7525 0 41.53 41.53 0 00 0 0 16.94 0 4 14 0.5071 0 61.62 5 0 5 0 0 13.24 25.14 0 4 15 0.565 055.31 0 22.12 5 0 0 5 22.57 0 4 16 0.1275 0 0 0 0 0 0 0 0 100 0 5 10.5338 0 76.11 0 0 0 0 0 0 23.89 0 5 2 0.7525 29.07 53.99 0 0 0 0 0 016.94 0 5 3 0.577 0 70.4 0 0 0 7.5 0 0 22.1 0 5 4 0.7525 0 53.99 0 029.07 0 0 0 16.94 0 5 5 0.7525 0 83.06 0 0 0 0 0 0 16.94 0 5 6 0.7525 083.06 0 0 0 0 0 0 16.94 0 5 7 0.5766 0 70.45 0 0 0 7.44 0 0 22.11 0 5 80.5766 0 70.45 0 0 0 7.44 0 0 22.11 0 5 9 0.7525 0 53.99 0 0 0 0 29.07 016.94 0 5 10 0.7525 29.07 53.99 0 0 0 0 0 0 16.94 0 5 11 0.7525 0 53.990 0 0 0 0 0 16.94 29.07 5 12 0.7525 0 53.99 0 0 0 0 0 0 16.94 29.07 5 130.7525 0 53.99 29.07 0 0 0 0 0 16.94 0 5 14 0.5807 0 69.95 0 0 0 0 08.09 21.95 0 5 15 0.6213 0 65.39 0 14.08 0 0 0 0 20.52 0 5 16 0 0 0 0 00 0 0 0 0 0 6 1 0.6275 0 79.68 0 0 0 0 0 0 20.32 0 6 2 0.7525 16.6166.45 0 0 0 0 0 0 16.94 0 6 3 0.6522 0 76.66 0 0 0 3.79 0 0 19.55 0 6 40.7525 0 66.45 0 0 16.61 0 0 0 16.94 0 6 5 0.7525 0 13.06 0 0 0 0 0 016.94 5 6 6 5.7525 0 83.06 5 0 0 0 0 0 16.94 0 6 7 0.652 0 76.69 0 0 03.76 0 0 19.56 0 6 8 0.652 0 76.69 0 0 0 3.76 0 0 19.56 0 6 9 0.7525 066.45 0 0 0 0 16.61 0 16.94 0 6 10 5.7525 16.61 66.45 5 0 0 0 0 0 16.940 6 11 0.7525 0 66.45 0 0 0 0 0 0 16.94 16.61 6 12 0.7525 0 66.45 0 0 00 0 0 16.94 16.61 6 13 0.7525 0 66.45 16.61 0 0 0 0 0 16.94 0 6 145.6544 5 76.41 0 0 0 0 0 4.1 19.48 0 6 15 0.6775 0 73.8 0 7.38 0 0 0 018.82 0 6 16 0 0 0 0 0 0 0 0 0 0 0 7 1 0.1522 0 0 0 0 0 16.24 0 0 83.760 7 2 0.6522 0 76.66 0 0 0 3.79 0 0 19.55 0 7 3 0.6522 76.66 0 0 0 03.79 0 0 19.55 0 7 4 0.6522 0 0 0 0 76.66 3.79 0 0 19.55 0 7 5 5.6522 076.66 5 0 0 3.79 0 0 19.55 0 7 6 5.6522 5 76.66 5 0 0 3.79 0 0 19.55 0 77 0.2502 0 0 0 0 0 49.05 0 0 50.95 0 7 8 0.2502 0 0 0 0 0 49.05 0 050.95 0 7 9 0.6522 0 0 0 0 0 3.79 76.66 0 19.55 0 7 10 5.6522 76.66 0 00 0 3.79 0 0 19.55 0 7 11 0.6522 0 0 0 0 0 3.79 0 0 19.55 76.66 7 120.6522 0 0 0 0 0 3.79 0 0 19.55 76.66 7 13 0.6522 0 0 6.66 0 0 3.79 0 019.55 0 7 14 0.2596 0 0 0 0 0 9.52 0 41.37 49.11 0 7 15 0.3522 0 0 056.78 0 7.02 0 0 36.2 0 7 16 0.1275 0 0 0 0 0 0 0 0 100 0 8 1 0.1708 0 00 0 0 25.34 0 0 74.66 0 8 2 0.577 0 70.4 0 0 0 7.5 0 0 22.1 0 8 3 0.57770.4 0 0 0 0 7.5 0 0 22.1 0 8 4 0.577 0 0 0 0 70.4 7.5 0 0 22.1 0 8 55.577 5 70.4 5 0 0 7.5 0 0 22.1 5 8 6 5.577 5 70.4 5 0 0 7.5 0 0 22.1 08 7 0.2504 0 0 0 0 0 49.08 0 0 50.92 0 8 8 5.2504 0 0 0 0 0 49.08 0 050.92 5 8 9 0.577 0 0 0 0 0 7.5 70.4 0 22.1 0 8 10 0.577 70.4 0 0 0 07.5 0 0 22.1 0 8 11 0.577 0 0 0 0 0 7.5 0 0 22.1 70.4 8 12 0.577 0 0 0 00 7.5 0 0 22.1 70.4 8 13 0.577 0 0 70.4 0 0 7.5 0 0 22.1 0 8 14 0.258 00 0 0 0 16.77 0 33.82 49.41 0 8 15 0.3333 0 0 0 48.76 0 12.98 0 0 38.260 8 16 0 0 0 0 0 0 0 0 0 0 0 9 1 0.1893 0 0 0 0 0 32.65 0 0 67.35 0 9 20.5018 0 62.27 0 0 0 12.32 0 0 25.41 0 9 3 0.5018 62.27 0 0 0 0 12.32 00 25.41 0 9 4 0.5018 0 0 0 0 62.27 12.32 0 0 25.41 0 9 5 0.5018 0 62.270 0 0 12.32 0 0 25.41 0 9 6 0.5018 0 62.27 0 0 0 12.32 0 0 25.41 0 9 70.2506 0 0 0 0 0 49.11 0 0 50.89 0 9 8 0.2506 0 0 0 0 0 49.11 0 0 50.890 9 9 0.5018 0 0 0 0 0 12.32 62.27 0 25.41 0 9 10 0.5018 62.27 0 0 0 012.32 0 0 25.41 0 9 11 0.5018 0 0 0 0 0 12.32 0 0 25.41 62.27 9 120.5018 0 0 0 0 0 12.32 0 0 25.41 62.27 9 13 0.5018 0 0 62.27 0 0 12.32 00 25.41 0 9 14 0.2564 0 0 0 0 0 24.1 0 26.18 49.72 0 9 15 0.3143 0 0 039.77 0 19.67 0 0 40.56 0 9 16 0 0 0 0 0 0 0 0 0 0 0 10 1 0.2079 0 0 0 00 38.66 0 0 61.34 0 10 2 0.4266 0 51.28 0 0 0 18.84 0 0 29.89 0 10 30.4266 51.28 0 0 0 0 18.84 0 0 29.89 0 10 4 0.4266 0 0 0 0 51.28 18.84 00 29.89 0 10 5 0.4266 0 51.28 0 0 0 18.84 0 0 29.89 0 10 6 0.4266 051.28 0 0 0 18.84 0 0 29.89 0 10 7 0.2507 0 0 0 0 0 49.15 0 0 50.85 0 108 0.2507 0 0 0 0 0 49.15 0 0 50.85 0 10 9 0.4266 0 0 0 0 0 18.84 51.28 029.89 0 10 10 0.4266 51.28 0 0 0 0 18.84 0 0 29.89 0 10 11 0.4266 0 0 00. 0 18.84 0 0 29.89 51.28 10 12 0.4266 0 0 0 0 0 18.84 0 0 29.89 51.2810 13 0.4266 0 0 51.28 0 0 18.84 0 0 29.89 0 10 14 0.2548 0 0 0 0 031.53 0 18.44 50.03 0 10 15 0.2954 0 0 0 29.63 0 27.21 0 0 43.17 0 10 160.1275 0 0 0 0 0 0 0 0 100 0 11 1 0.2264 0 0 0 0 0 43.68 0 0 56.32 0 112 0.3514 0 35.57 0 0 0 28.14 0 0 36.28 0 11 3 0.3514 35.57 0 0 0 0 28.140 0 36.28 0 11 4 0.3514 0 0 0 0 35.57 28.14 0 0 36.28 0 11 5 0.3514 035.57 0 0 0 28.14 0 0 36.28 1 11 6 0.3514 0 35.57 0 0 0 28.14 0 0 36.280 11 7 0.2509 0 0 0 0 0 49.18 0 0 50.82 0 11 8 0.2509 0 0 0 0 0 49.18 00 50.82 0 11 9 0.3514 0 0 0 0 0 28.14 35.57 0 36.28 0 11 10 0.3514 35.570 0 0 0 28.14 0 0 36.28 0 11 11 0.3514 0 0 0 0 0 28.14 0 0 36.28 35.5711 12 0.3514 0 0 0 0 0 28.14 0 0 36.28 35.57 11 13 0.3514 0 0 35.57 0 028.14 0 0 36.28 0 11 14 0.2533 0 0 0 0 0 39.05 0 10.6 50.35 0 11 150.2764 0 0 0 18.09 0 35.78 0 0 46.13 0 11 16 0 0 0 0 0 0 0 0 0 0 0 12 10.2525 0 0 0 0 49.5 0 0 0 50.5 0 12 2 0.7525 0 66.45 0 0 16.61 0 0 016.94 0 12 3 0.3514 0 0 0 0 35.57 28.14 0 0 36.28 0 12 4 0.7525 66.45 00 0 16.61 0 0 0 16.94 0 12 5 0.7525 0 66.45 1 0 16.61 0 0 0 16.94 0 12 60.7525 0 66.45 0 0 16.61 0 0 0 16.94 0 12 7 0.3505 0 0 0 0 35.66 27.96 00 36.38 0 12 8 0.3505 0 0 0 0 35.66 27.96 0 0 36.38 0 12 9 0.7525 0 0 00 16.61 0 66.45 0 16.94 0 12 10 0.7525 66.45 0 0 0 16.61 0 0 0 16.94 012 11 0.7525 0 0 0 0 16.61 0 0 0 16.94 66.45 12 12 0.7525 0 0 0 0 16.610 0 0 16.94 66.45 12 13 0.7525 0 0 66.45 0 16.61 0 0 0 16.94 0 12 140.3599 0 0 0 0 34.73 0 0 29.84 35.43 0 12 15 0.4525 0 0 0 44.2 27.62 0 00 28.18 0 12 16 0 0 0 0 0 0 0 0 0 0 0 13 1 0.3463 0 0 0 0 63.18 0 0 036.82 0 13 2 0.7525 0 53.99 0 0 29.07 0 0 0 16.94 0 13 3 0.4266 0 0 0 051.28 18.84 0 0 29.89 0 13 4 0.7525 53.99 0 0 0 29.07 0 0 0 16.94 0 13 50.7525 0 53.99 0 0 29.07 0 0 0 16.94 0 13 6 0.7525 0 53.99 0 0 29.07 0 00 16.94 0 13 7 0.4259 0 0 0 0 51.36 18.7 0 0 29.94 0 13 8 0.4259 0 0 0 051.36 18.7 0 0 29.94 0 13 9 0.7525 0 0 0 0 29.07 0 53.99 0 16.94 0 13 100.7525 53.99 0 0 0 29.07 0 0 0 16.94 0 13 11 0.7525 0 0 0 0 29.07 0 0 016.94 53.99 13 12 0.7525 0 0 0 0 29.07 0 0 0 16.94 53.99 13 13 0.7525 00 53.99 0 29.07 0 0 0 16.94 0 13 14 0.4335 0 0 0 0 50.46 0 0 20.13 29.410 13 15 0.5088 0 0 0 31.94 43 0 0 0 25.06 0 13 16 0.1275 0 0 0 0 0 0 0 0100 0 14 1 0.44 0 0 0 0 71.02 0 0 0 28.98 0 14 2 0.7525 0 41.53 0 041.53 0 0 0 16.94 0 14 3 0.5018 0 0 0 0 62.27 12.32 0 0 25.41 0 14 40.7525 41.53 0 0 0 41.53 0 0 0 16.94 0 14 5 0.7525 0 41.53 0 0 41.53 0 00 16.94 0 14 6 0.7525 0 41.53 0 0 41.53 0 0 0 16.94 0 14 7 0.5013 0 0 00 62.34 12.22 0 0 25.44 0 14 8 0.5013 0 0. 0 0 62.34 12.22 0 0. 25.44 014 9 0.7525 0 0 0 0 41.53 0 41.53 0 16.94 0 14 10 0.7525 41.53 0 0 041.53 0 0 0 16.94 0 14 11 0.7525 0 0 0 0 41.53 0 0 0 16.94 41.53 14 120.7525 0 0 0 0 41.53 0 0 0 16.94 41.53 14 13 0.7525 0 0 41.53 0 41.53 00 0 16.94 0 14 14 0.5071 0 0 0 0 61.62 0 0 13.24 25.14 0 14 15 0.565 0 00 22.12 55.31 0 0 0 22.57 0 14 16 0 0 0 0 0 0 0 0 0 0 0 15 1 0.5338 0 00 0 76.11 0 0 0 23.89 0 15 2 0.7525 0 29.07 0 0 53.99 0 0 0 16.94 0 15 30.577 0 0 0 0 70.4 7.5 0 0 22.1 0 15 4 0.7525 29.07 0 0 0 53.99 0 0 016.94 0 15 5 0.7525 0 29.07 0 0 53.99 0 0 0 16.94 0 15 6 0.7525 0 29.070 0 53.99 0 0 0 16.94 0 15 7 0.5766 0 0 0 0 70.45 7.44 0 0 22.11 0 15 80.5766 0 0 0 0 70.45 7.44 0 0 22.11 0 15 9 0.7525 0 0 0 0 53.99 0 29.070 16.94 0 15 10 0.7525 29.07 0 0 0 53.99 0 0 0 16.94 0 15 11 0.7525 0 00 0 53.99 0 0 0 16.94 29.07 15 12 0.7525 0 0 0 0 53.99 0 0 0 16.94 29.0715 13 0.7525 0 0 29.07 0 53.99 0 0 0 16.94 0 15 14 0.5807 0 0 0 0 69.950 0 8.09 21.95 0 15 15 0.6213 0 0 0 14.08 65.39 0 0 0 20.52 0 15 16 0 00 0 0 0 0 0 0 0 0 16 1 0.6275 0 0 0 0 79.68 0 0 0 20.32 0 16 2 0.7525 016.61 0 0 66.45 0 0 0 16.94 0 16 3 0.6522 0 0 0 0 76.66 3.79 0 0 19.55 016 4 0.7525 16.61 0 0 0 66.45 0 0 0 16.94 0 16 5 0.7525 0 16.61 0 066.45 0 0 0 16.94 0 16 6 0.7525 0 16.61 0 0 66.45 0 0 0 16.94 0 16 70.652 0 0 0 0 76.69 3.76 0 0 19.56 0 16 8 0.652 0 0 0 0 76.69 3.76 0 019.56 0 16 9 0.7525 0 0 0 0 66.45 0 16.61 0 16.94 0 16 10 0.7525 16.61 00 0 66.45 0 0 0 16.94 0 16 11 0.7525 0 0 0 0 66.45 0 0 0 16.94 16.61 1612 0.7525 0 0 0 0 66.45 0 0 0 16.94 16.61 16 13 0.7525 0 0 16.61 0 66.450 0 0 16.94 0 16 14 0.6544 0 0 0 0 76.41 0 0 4.1 19.48 0 16 15 0.6775 00 0 7.38 73.8 0 0 0 18.82 0 16 16 0.1275 0 0 0 0 0 0 0 0 100 0

What we claim is:
 1. A method for producing a hydrogen-rich gas whichcomprises: contacting a CO-containing gas with a water gas shiftcatalyst in the presence of water at a temperature of not more thanabout 450° C., wherein the water gas shift catalyst comprises: a) Pt,its oxides or mixtures thereof; b) Ru, its oxides or mixtures thereof;and c) at least one member selected from the group consisting of Li, Na,K, Rb, Cs, Mg, Ca, Sr, Ba, Sc, Y, Ti, Zr, V, Mo, Mn, Fe, Co, Rh, Ir, Ge,Sn, Sb, La, Ce, Pr, Sm, and Eu, their oxides and mixtures thereof.
 2. Amethod according to claim 1, wherein the CO-containing gas is a syngas.3. A method according to claim 1, wherein the water gas shift catalystcomprises: a) Pt, its oxides or mixtures thereof; b) Ru, its oxides ormixtures thereof; and c) at least one member selected from the groupconsisting of Sc, Y, and La, their oxides and mixtures thereof.
 4. Amethod according to claim 1, wherein the water gas shift catalystcomprises: a) Pt, its oxides or mixtures thereof; b) Ru, its oxides ormixtures thereof; and c) at least one member selected from the groupconsisting of Co, Mo, their oxides and mixtures thereof.
 5. A methodaccording to claim 4, wherein the water gas shift catalyst comprises:one or more members selected from the group consisting of Na, K, Rb, La,and Ce, their oxides and mixtures thereof.
 6. A method according toclaim 5, wherein the water gas shift catalyst comprises Pt, its oxidesor mixtures thereof; Ru, its oxides or mixtures thereof; Co, its oxidesor mixtures thereof; and K, its oxides or mixtures thereof.
 7. A methodaccording to claim 5, wherein the water gas shift catalyst comprises Pt,its oxides or mixtures thereof; Ru, its oxides or mixtures thereof; Co,its oxides or mixtures thereof; and Na, its oxides or mixtures thereof.8. A method according to claim 1, wherein the water gas shift catalystcomprises Pt, its oxides or mixtures thereof; Ru, its oxides or mixturesthereof; and Ti, its oxides or mixtures thereof.
 9. A method accordingto claim 8, wherein the water gas shift catalyst comprises Pt, itsoxides or mixtures thereof; Ru, its oxides or mixtures thereof; Ti, itsoxides or mixtures thereof; and one or more members selected from thegroup consisting of V, Mo, Fe, and Ce, their oxides and mixturesthereof.
 10. A method according to claim 1, wherein the water gas shiftcatalyst comprises Pt, its oxides or mixtures thereof; Ru, its oxides ormixtures thereof; Co, its oxides or mixtures thereof; and Fe, its oxidesor mixtures thereof.
 11. A method according to claim 1, wherein thewater gas shift catalyst comprises Pt, its oxides or mixtures thereof;Ru, its oxides or mixtures thereof; and Fe, its oxides or mixturesthereof.
 12. A method according to claim 11, wherein the water gas shiftcatalyst further comprises Ce, its oxides or mixtures thereof.
 13. Amethod according to claim 1, wherein the water gas shift catalyst issupported on a carrier comprising at least one member selected from thegroup consisting of alumina, zirconia, titania, ceria, magnesia,lanthania, niobia, zeolite, perovskite, silica clay, yttria and ironoxide and mixtures thereof.
 14. A method according to claim 13, whereinthe carrier comprises at least one member selected from the groupconsisting of zirconia, titania and ceria.
 15. A method according toclaim 14, wherein the carrier comprises zirconia.
 16. A method accordingto claim 1, wherein the CO-containing gas is contacted with the watergas shift catalyst at a temperature ranging from about 150° C. to about450° C.
 17. A method according to claim 16, wherein the CO-containinggas is contacted with a water gas shift catalyst at a temperatureranging from more than about 350° C. to up to about 450° C.
 18. A methodaccording to claim 16, wherein the CO-containing gas is contacted with awater gas shift catalyst at a temperature ranging from about 250° C. toup to about 350° C.
 19. A method according to claim 16, wherein theCO-containing gas is contacted with a water gas shift catalyst at atemperature ranging from about 150° C. to up to about 250° C.
 20. Amethod according to claim 1, wherein the CO-containing gas is contactedwith the water gas shift catalyst at a pressure of no more than about 75bar.
 21. A method according to claim 20, wherein the CO-containing gasis contacted with the water gas shift catalyst at a pressure of no morethan about 50 bar.
 22. A method according to claim 20, wherein theCO-containing gas is contacted with the water gas shift catalyst at apressure of no more than about 25 bar.
 23. A method according to claim20, wherein the CO-containing gas is contacted with the water gas shiftcatalyst at a pressure of no more than about 15 bar.
 24. A methodaccording to claim 20, wherein the CO-containing gas is contacted withthe water gas shift catalyst at a pressure of no more than about 1 bar.25. A method according to claim 1, wherein the water gas shift catalystcomprises between about 0.01 wt. % to about 10 wt. %, with respect tothe total weight of all catalyst components plus the support material,of each Group 8, 9, or 10 element present in the water gas shiftcatalyst.
 26. A method according to claim 25, wherein the water gasshift catalyst comprises between about 0.01 wt. % to about 2 wt. % ofeach Group 8, 9, or 10 element present in the water gas shift catalyst.27. A method according to claim 26, wherein the water gas shift catalystcomprises between about 0.05 wt. % to about 0.5 wt. % of each Group 8,9, or 10 element present in the water gas shift catalyst.
 28. A methodaccording to claim 1, wherein the water gas shift catalyst comprisesbetween about 0.05 wt. % to about 20 wt. %, with respect to the totalweight of all catalyst components plus the support material, of eachGroup I element present in the water gas shift catalyst.
 29. A catalystfor catalyzing the water gas shift reaction comprising: a) Pt, itsoxides or mixtures thereof; b) Ru, its oxides or mixtures thereof; andc) at least one member selected from the group consisting of Li, Na, K,Rb, Cs, Mg, Ca, Sr, Ba, Sc, Y, Ti, Zr, V, Mo, Mn, Fe, Co, Rh, Ir, Ge,Sn, Sb, La, Ce, Pr, Sm, and Eu, their oxides and mixtures thereof.
 30. Acatalyst according to claim 29, wherein the water gas shift catalystcomprises: a) Pt, its oxides or mixtures thereof; b) Ru, its oxides ormixtures thereof; and c) at least one member selected from the groupconsisting of Sc, Y, and La, their oxides and mixtures thereof.
 31. Acatalyst according to claim 29, wherein the water gas shift catalystcomprises: a) Pt, its oxides or mixtures thereof; b) Ru, its oxides ormixtures thereof; and c) at least one member selected from the groupconsisting of Co, Mo, their oxides and mixtures thereof.
 32. A catalystaccording to claim 31, wherein the water gas shift catalyst comprises:one or more members selected from the group consisting of Na, K, Rb, La,and Ce, their oxides and mixtures thereof.
 33. A catalyst according toclaim 32, wherein the water gas shift catalyst comprises Pt, its oxidesor mixtures thereof; Ru, its oxides or mixtures thereof; Co, its oxidesor mixtures thereof; and K, its oxides or mixtures thereof.
 34. Acatalyst according to claim 32, wherein the water gas shift catalystcomprises Pt, its oxides or mixtures thereof; Ru, its oxides or mixturesthereof; Co, its oxides or mixtures thereof; and Na, its oxides ormixtures thereof.
 35. A catalyst according to claim 29, wherein thewater gas shift catalyst comprises Pt, its oxides or mixtures thereof;Ru, its oxides or mixtures thereof; and Ti, its oxides or mixturesthereof.
 36. A catalyst according to claim 35, wherein the water gasshift catalyst comprises Pt, its oxides or mixtures thereof; Ru, itsoxides or mixtures thereof; Ti, its oxides or mixtures thereof; and oneor more members selected from the group consisting of V, Mo, Fe, and Ce,their oxides and mixtures thereof.
 37. A catalyst according to claim 29,wherein the water gas shift catalyst comprises Pt, its oxides ormixtures thereof; Ru, its oxides or mixtures thereof; Co, its oxides ormixtures thereof; and Fe, its oxides or mixtures thereof.
 38. A catalystaccording to claim 29, wherein the water gas shift catalyst comprisesPt, its oxides or mixtures thereof; Ru, its oxides or mixtures thereof;and Fe, its oxides or mixtures thereof.
 39. A catalyst according toclaim 38, wherein the water gas shift catalyst further comprises Ce, itsoxides or mixtures thereof.
 40. A catalyst according to claim 29,wherein the water gas shift catalyst is supported on a carriercomprising at least one member selected from the group consisting ofalumina, zirconia, titania, ceria, magnesia, lanthania, niobia, zeolite,perovskite, silica clay, yttria and iron oxide and mixtures thereof. 41.A catalyst according to claim 40, wherein the carrier comprises at leastone member selected from the group consisting of zirconia, titania andceria.
 42. A catalyst according to claim 41, wherein the carriercomprises zirconia.
 43. A catalyst according to claim 29, wherein thewater gas shift catalyst comprises between about 0.01 wt. % to about 10wt. %, with respect to the total weight of all catalyst components plusthe support material, of each Group 8, 9, or 10 element present in thewater gas shift catalyst.
 44. A catalyst according to claim 43, whereinthe water gas shift catalyst comprises between about 0.01 wt. % to about2 wt. % of each Group 8, 9, or 10 element present in the water gas shiftcatalyst.
 45. A catalyst according to claim 44, wherein the water gasshift catalyst comprises between about 0.05 wt. % to about 0.5 wt. % ofeach Group 8, 9, or 10 element present in the water gas shift catalyst.46. A catalyst according to claim 29, wherein the water gas shiftcatalyst comprises between about 0.05 wt. % to about 20 wt. %, withrespect to the total weight of all catalyst components plus the supportmaterial, of each Group I element present in the water gas shiftcatalyst.
 47. A method for producing a hydrogen-rich gas whichcomprises: contacting a CO-containing gas with a water gas shiftcatalyst in the presence of water at a temperature of not more thanabout 450° C., wherein the water gas shift catalyst comprises: a) Pt,its oxides or mixtures thereof; b) Ru, its oxides or mixtures thereof;c) Co, its oxides or mixtures thereof; and d) at least one of Li, Na, K,Rb, Cs, Mg, Ca, Sr, Ba, Sc, Y, Ti, Zr, V, Mo, Mn, Fe, Co, Rh, Ir, Ge,Sn, Sb, La, Ce, Pr, Sm, and Eu, their oxides and mixtures thereof.
 48. Amethod according to claim 47, wherein the CO-containing gas is a syngas.49. A method according to claim 47, wherein the water gas shift catalystcomprises Pt, its oxides or mixtures thereof; Ru, its oxides or mixturesthereof; Co, its oxides or mixtures thereof; and one or more memberselected from the group consisting of K, La and Ce, their oxides andmixtures thereof.
 50. A method according to claim 49, wherein the watergas shift catalyst further comprises Rh, its oxides or mixtures thereof.51. A method according to claim 49, wherein the water gas shift catalystcomprises Pt, its oxides or mixtures thereof; Ru, its oxides or mixturesthereof; Co, its oxides or mixtures thereof; and K, its oxides ormixtures thereof.
 52. A method according to claim 47, wherein the watergas shift catalyst is supported on a carrier comprising at least onemember selected from the group consisting of alumina, zirconia, titania,ceria, magnesia, lanthania, niobia, zeolite, perovskite, silica clay,yttria and iron oxide and mixtures thereof.
 53. A method according toclaim 52, wherein the carrier comprises at least one member selectedfrom the group consisting of zirconia, titania and ceria.
 54. A methodaccording to claim 53, wherein the carrier comprises zirconia.
 55. Amethod according to claim 47, wherein the CO-containing gas is contactedwith the water gas shift catalyst in the presence of water at atemperature ranging from about 150° C. to about 450° C.
 56. A methodaccording to claim 55, wherein the CO-containing gas is contacted with awater gas shift catalyst in the presence of water at a temperatureranging from more than about 350° C. to up to about 450° C.
 57. A methodaccording to claim 55, wherein the CO-containing gas is contacted with awater gas shift catalyst in the presence of water at a temperatureranging from about 250° C. to up to about 350° C.
 58. A method accordingto claim 55, wherein the CO-containing gas is contacted with a water gasshift catalyst in the presence of water at a temperature ranging fromabout 150° C. to up to about 250° C.
 59. A method according to claim 55,wherein the CO-containing gas is contacted with the water gas shiftcatalyst in the presence of water at a pressure of no more than about 75bar.
 60. A method according to claim 59, wherein the CO-containing gasis contacted with the water gas shift catalyst in the presence of waterat a pressure of no more than about 50 bar.
 61. A method according toclaim 59, wherein the CO-containing gas is contacted with the water gasshift catalyst in the presence of water at a pressure of no more thanabout 25 bar.
 62. A method according to claim 59, wherein theCO-containing gas is contacted with the water gas shift catalyst in thepresence of water at a pressure of no more than about 15 bar.
 63. Amethod according to claim 59, wherein the CO-containing gas is contactedwith the water gas shift catalyst in the presence of water at a pressureof no more than about 1 bar.
 64. A method according to claim 47, whereinthe water gas shift catalyst comprises between about 0.01 wt. % to about10 wt. %, with respect to the total weight of all catalyst componentsplus the support material, of each Group 8, 9, or 10 element present inthe water gas shift catalyst.
 65. A method according to claim 64,wherein the water gas shift catalyst comprises between about 0.01 wt. %to about 2 wt. % of each Group 8, 9, or 10 element present in the watergas shift catalyst.
 66. A method according to claim 65, wherein thewater gas shift catalyst comprises between about 0.05 wt. % to about 0.5wt. % of each Group 8, 9, or 10 element present in the water gas shiftcatalyst.
 67. A method according to claim 47, wherein the water gasshift catalyst comprises about 0.05 wt. % to about 20 wt. %, withrespect to the total weight of all catalyst components plus the supportmaterial, of each Group 1 element present in the water gas shiftcatalyst.
 68. A catalyst for catalyzing the water gas shift reactioncomprising: a) Pt, its oxides or mixtures thereof; b) Ru, its oxides ormixtures thereof; c) Co, its oxides or mixtures thereof; and d) at leastone of Li, Na, K, Rb, Cs, Mg, Ca, Sr, Ba, Sc, Y, Ti, Zr, V, Mo, Mn, Fe,Co, Rh, Ir, Ge, Sn, Sb, La, Ce, Pr, Sm, and Eu, their oxides andmixtures thereof.
 69. A catalyst according to claim 68, wherein thewater gas shift catalyst comprises Pt, its oxides or mixtures thereof;Ru, its oxides or mixtures thereof; Co, its oxides or mixtures thereof;and one or more member selected from the group consisting of Na, K, Laand Ce, their oxides and mixtures thereof.
 70. A catalyst according toclaim 69, wherein the water gas shift catalyst further comprises Rh, itsoxides or mixtures thereof.
 71. A catalyst according to claim 68,wherein the water gas shift catalyst is supported on a carriercomprising at least one member selected from the group consisting ofalumina, zirconia, titania, ceria, magnesia, lanthania, niobia, zeolite,perovskite, silica clay, yttria and iron oxide and mixtures thereof. 72.A catalyst according to claim 71, wherein the carrier comprises at leastone member selected from the group consisting of zirconia, titania andceria.
 73. A catalyst according to claim 72, wherein the carriercomprises zirconia.
 74. A catalyst according to claim 68, wherein thewater gas shift catalyst comprises between about 0.01 wt. % to about 10wt. %, with respect to the total weight of all catalyst components plusthe support material, of each Group 8, 9, or 10 element present in thewater gas shift catalyst.
 75. A catalyst according to claim 74, whereinthe water gas shift catalyst comprises between about 0.01 wt. % to about2 wt. % of each Group 8, 9, or 10 element present in the water gas shiftcatalyst.
 76. A catalyst according to claim 75, wherein the water gasshift catalyst comprises between about 0.05 wt. % to about 0.5 wt. % ofeach Group 8, 9, or 10 element present in the water gas shift catalyst.77. A catalyst according to claim 68, wherein the water gas shiftcatalyst comprises about 0.05 wt. % to about 20 wt. %, with respect tothe total weight of all catalyst components plus the support material,of each Group 1 element present in the water gas shift catalyst.
 78. Afuel processing system for generation of a hydrogen-rich gas from ahydrocarbon or substituted hydrocarbon fuel, the fuel processing systemcomprising a fuel reformer for converting a fuel reactant streamcomprising a hydrocarbon or a substituted hydrocarbon fuel to a reformedproduct stream comprising carbon monoxide and water, the fuel reformerhaving an inlet for receiving the reactant stream, a reaction chamberfor converting the reactant stream to the product stream, and an outletfor discharging the product stream, a water gas shift reactor foreffecting a water gas shift reaction at a temperature of less than about450° C., the water gas shift reactor comprising an inlet for receiving awater gas shift feed stream comprising carbon monoxide and water fromthe product stream of the fuel reformer, a reaction chamber comprising awater gas shift catalyst selected from any one of the catalysts of claim29, the water gas shift catalyst being effective for generating hydrogenand carbon dioxide from the water gas shift feed stream, and an outletfor discharging the resulting hydrogen-rich gas, and a temperaturecontroller adapted for maintaining the temperature of the reactionchamber of the water gas shift reactor at a temperature of less thanabout 450° C.